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  <front>
    <journal-meta><journal-id journal-id-type="publisher">ESSD</journal-id><journal-title-group>
    <journal-title>Earth System Science Data</journal-title>
    <abbrev-journal-title abbrev-type="publisher">ESSD</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">Earth Syst. Sci. Data</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">1866-3516</issn><publisher>
    <publisher-name>Copernicus Publications</publisher-name>
    <publisher-loc>Göttingen, Germany</publisher-loc>
  </publisher></journal-meta>
    <article-meta>
      <article-id pub-id-type="doi">10.5194/essd-18-4793-2026</article-id><title-group><article-title>A global dataset of <inline-formula><mml:math id="M1" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M2" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M3" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures and associated uncertainties (1998–2022), with a sensitivity analysis to support isotopic inversions</article-title><alt-title><inline-formula><mml:math id="M4" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M5" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M6" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> uncertainty analysis</alt-title>
      </title-group>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Tapin</surname><given-names>Emeline</given-names></name>
          <email>emeline.tapin@lsce.ipsl.fr</email>
        <ext-link>https://orcid.org/0009-0009-2345-1182</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Berchet</surname><given-names>Antoine</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6709-0125</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Martinez</surname><given-names>Adrien</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-8508-9005</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff6">
          <name><surname>Menoud</surname><given-names>Malika</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-7061-2684</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2">
          <name><surname>Thanwerdas</surname><given-names>Joël</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-1040-831X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3 aff4">
          <name><surname>Lan</surname><given-names>Xin</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6327-6950</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>Malina</surname><given-names>Edward</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1055-4598</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>Gasbarra</surname><given-names>Daniele</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Saunois</surname><given-names>Marielle</given-names></name>
          
        </contrib>
        <aff id="aff1"><label>1</label><institution>Laboratoire des Sciences du Climat et de l'Environnement (LSCE), CEA, CNRS, UVSQ, Université Paris-Saclay, Gif-sur-Yvette, France</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Empa, Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, Switzerland</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>CIRES, University of Colorado Boulder, CO, 80309, USA</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>NOAA Global Monitoring Laboratory, Boulder, CO, 80305, USA</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>European Space Agency  –  ESRIN, Frascati, 00044, Italy</institution>
        </aff>
        <aff id="aff6"><label>a</label><institution>now at: UNEP, International Methane Emissions Observatory (IMEO), Paris, France</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Emeline Tapin (emeline.tapin@lsce.ipsl.fr)</corresp></author-notes><pub-date><day>10</day><month>July</month><year>2026</year></pub-date>
      
      <volume>18</volume>
      <issue>7</issue>
      <fpage>4793</fpage><lpage>4832</lpage>
      <history>
        <date date-type="received"><day>7</day><month>November</month><year>2025</year></date>
           <date date-type="rev-request"><day>13</day><month>February</month><year>2026</year></date>
           <date date-type="rev-recd"><day>27</day><month>May</month><year>2026</year></date>
           <date date-type="accepted"><day>12</day><month>June</month><year>2026</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2026 Emeline Tapin et al.</copyright-statement>
        <copyright-year>2026</copyright-year>
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026.html">This article is available from https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026.html</self-uri><self-uri xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026.pdf">The full text article is available as a PDF file from https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d2e247">The isotopic composition of atmospheric methane (<inline-formula><mml:math id="M7" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M8" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M9" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) provides critical constraints for attributing methane emissions to specific sources. In this study, we present updated global maps of <inline-formula><mml:math id="M10" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M11" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M12" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures across five major methane-emitting sectors (fossil fuels and geological, agriculture and waste, biomass and biofuel burning, wetlands, and other natural sources) for the period 1998–2022. These maps integrate recent spatially explicit datasets and literature-derived observations, and include explicit quantification of both intrinsic (within-sector) and aggregation-related uncertainties. Building upon previous global compilations, our dataset extends the temporal coverage to 2022, harmonizes sectoral definitions with the Global Methane Budget framework, and provides a consistent and traceable quantification of uncertainties suitable for atmospheric inversions. We assess the influence of these updated source signatures on the modeled atmospheric <inline-formula><mml:math id="M13" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M14" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M15" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> using forward simulations within the Community Inversion Framework (CIF) coupled to the LMDz transport model. A comprehensive sensitivity analysis quantifies the impacts of key drivers of uncertainty, including emission flux datasets, OH sinks, kinetic isotope effects, and isotopic source signatures. We show that uncertainties in methane oxidation chemistry and source signatures, particularly from agriculture and waste, dominate the variability in the modeled <inline-formula><mml:math id="M16" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M17" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M18" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal, while the impact of flux aggregation choices is comparatively minor. The updated isotopic dataset is provided on a global <inline-formula><mml:math id="M19" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mi mathvariant="italic">°</mml:mi><mml:mo>×</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mi mathvariant="italic">°</mml:mi></mml:mrow></mml:math></inline-formula> grid, supporting future atmospheric inversions and improved methane budget assessments at global and regional scales. Practical guidelines for configuring isotopic inversions, including recommended uncertainty specifications and key parameters to optimize, are also provided, offering a framework for next-generation <inline-formula><mml:math id="M20" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M21" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M22" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> inversion studies. The final version of the gridded <inline-formula><mml:math id="M23" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M24" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M25" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature dataset is available under CC BY 4.0 (<xref ref-type="bibr" rid="bib1.bibx133" id="altparen.1"/>,  <ext-link xlink:href="https://doi.org/10.57780/ESA-6D202E9" ext-link-type="DOI">10.57780/ESA-6D202E9</ext-link>).</p>
  </abstract>
    
<funding-group>
<award-group id="gs1">
<funding-source>European Space Agency</funding-source>
<award-id>4000142730/23/I-NS</award-id>
</award-group>
</funding-group>
</article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d2e458">Methane (<inline-formula><mml:math id="M26" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) is the second most significant anthropogenic greenhouse gas after carbon dioxide (<inline-formula><mml:math id="M27" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>), playing a major role in current climate change <xref ref-type="bibr" rid="bib1.bibx130 bib1.bibx30" id="paren.2"/>. Its atmospheric concentration has more than doubled since pre-industrial times, to reach 1946 <inline-formula><mml:math id="M28" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> in November 2025 <xref ref-type="bibr" rid="bib1.bibx30 bib1.bibx58" id="paren.3"/>. Despite its lower abundance compared to <inline-formula><mml:math id="M29" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M30" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> has contributed approximately 31 <inline-formula><mml:math id="M31" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> (1.19 <inline-formula><mml:math id="M32" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">W</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) of the total radiative forcing from anthropogenic greenhouse gases since 1750 <xref ref-type="bibr" rid="bib1.bibx30" id="paren.4"/>, owing to its high global warming potential (GWP: 29.8 over 100 <inline-formula><mml:math id="M33" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">years</mml:mi></mml:mrow></mml:math></inline-formula>, 82.5 over 20 <inline-formula><mml:math id="M34" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">years</mml:mi></mml:mrow></mml:math></inline-formula>). Its relatively short atmospheric lifetime (about 9 <inline-formula><mml:math id="M35" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">years</mml:mi></mml:mrow></mml:math></inline-formula> for the burden; <xref ref-type="bibr" rid="bib1.bibx98" id="altparen.5"/>, and approximately 12 <inline-formula><mml:math id="M36" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">years</mml:mi></mml:mrow></mml:math></inline-formula> for the perturbation lifetime <xref ref-type="bibr" rid="bib1.bibx30" id="altparen.6"/>) compared to <inline-formula><mml:math id="M37" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> makes it an effective target for near-term climate mitigation strategies <xref ref-type="bibr" rid="bib1.bibx88 bib1.bibx124" id="paren.7"/>. Global initiatives such as the Global Methane Pledge (launched at COP26) aim to reduce global anthropogenic methane emissions by 30 <inline-formula><mml:math id="M38" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> by 2030 compared to 2020 levels <xref ref-type="bibr" rid="bib1.bibx37 bib1.bibx140" id="paren.8"/>. After a stabilization phase between 1999–2006, atmospheric <inline-formula><mml:math id="M39" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> resumed its growth after 2007, diverging from trajectories compatible with the Paris Agreement <xref ref-type="bibr" rid="bib1.bibx84" id="paren.9"/>. This renewed increase remains a subject of active scientific debate <xref ref-type="bibr" rid="bib1.bibx119 bib1.bibx114 bib1.bibx83 bib1.bibx84 bib1.bibx104 bib1.bibx109 bib1.bibx149 bib1.bibx70 bib1.bibx137 bib1.bibx113 bib1.bibx139 bib1.bibx33 bib1.bibx153 bib1.bibx48 bib1.bibx3 bib1.bibx17 bib1.bibx136 bib1.bibx34 bib1.bibx103" id="paren.10"/>, and highlights the urgent need to better constrain methane sources and sinks <xref ref-type="bibr" rid="bib1.bibx109 bib1.bibx110 bib1.bibx111" id="paren.11"><named-content content-type="pre">e.g.</named-content></xref>. Since 2020, the growth of atmospheric <inline-formula><mml:math id="M40" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> has further accelerated, with unprecedented annual increases recorded between 2020–2022 <xref ref-type="bibr" rid="bib1.bibx75 bib1.bibx49 bib1.bibx21" id="paren.12"/>.</p>
      <p id="d2e650">Methane emissions have both natural (around 200 <inline-formula><mml:math id="M41" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, e.g. wetlands, freshwaters, geological sources, natural wildfires) and anthropogenic origins (around 320 <inline-formula><mml:math id="M42" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, e.g. agriculture, fossil fuel, waste, and anthropogenic biomass and biofuel burning) <xref ref-type="bibr" rid="bib1.bibx111" id="paren.13"/>. However, large uncertainties persist in the relative contributions of these sources. <inline-formula><mml:math id="M43" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> fluxes can be estimated using two main approaches: bottom-up and top-down methods. Bottom-up methods use either emission inventories derived from sectoral activity data and emission factors, or process-based models <xref ref-type="bibr" rid="bib1.bibx111" id="paren.14"/>. While they offer detailed source-level information, these estimates are not directly constrained by atmospheric observations and often lead to budgets that are inconsistent with the atmospheric <inline-formula><mml:math id="M44" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> burden. In contrast, top-down methods rely on atmospheric measurements of <inline-formula><mml:math id="M45" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, including in situ observations from ground-based stations and remote sensing data from satellites, combined with transport models (e.g. LMDZ) to statistically optimize emissions. These approaches are global and observation-based but often struggle to attribute emissions to specific sources when those are co-located or have overlapping temporal signals <xref ref-type="bibr" rid="bib1.bibx46 bib1.bibx8" id="paren.15"/>. They can also face regional attribution challenges, particularly in areas with sparse or uneven observational coverage <xref ref-type="bibr" rid="bib1.bibx110 bib1.bibx111" id="paren.16"/>. The discrepancies between these two methods, in both magnitude and spatial distribution, highlight major gaps in our understanding of <inline-formula><mml:math id="M46" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> sources and sinks <xref ref-type="bibr" rid="bib1.bibx111" id="paren.17"/>. Accurately attributing atmospheric <inline-formula><mml:math id="M47" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> to specific formation processes can be difficult, especially when co-located sources cannot be differentiated using <inline-formula><mml:math id="M48" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mixing ratios or their spatial and seasonal variability <xref ref-type="bibr" rid="bib1.bibx6 bib1.bibx7 bib1.bibx52 bib1.bibx109" id="paren.18"/>. Yet the quantification of individual methane sources is required to implement effective mitigation strategies.</p>
      <p id="d2e785">The isotopic composition of methane, particularly the ratio of <inline-formula><mml:math id="M49" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M50" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>, can be used for source attribution because it depends on the formation pathway <xref ref-type="bibr" rid="bib1.bibx122 bib1.bibx56" id="paren.19"><named-content content-type="pre">e.g.</named-content></xref>. It is expressed as <inline-formula><mml:math id="M51" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M52" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M53" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>:

              <disp-formula id="Ch1.E1" content-type="numbered"><label>1</label><mml:math id="M54" display="block"><mml:mstyle class="stylechange" displaystyle="true"/><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mi mathvariant="italic">δ</mml:mi><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow><mml:mtext>-</mml:mtext><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow><mml:mo>=</mml:mo><mml:mfenced close=")" open="("><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mfenced open="(" close=")"><mml:mrow><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi><mml:msup><mml:mo>/</mml:mo><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:mfenced><mml:mtext>sample</mml:mtext></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mi>R</mml:mi><mml:mtext>VPDB</mml:mtext></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:mfenced><mml:mo>×</mml:mo><mml:mn mathvariant="normal">1000</mml:mn><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>

        where <inline-formula><mml:math id="M55" display="inline"><mml:mrow><mml:mfenced open="(" close=")"><mml:mrow><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi><mml:msup><mml:mo>/</mml:mo><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:mfenced></mml:mrow></mml:math></inline-formula> denotes the ratio of molar quantities of <inline-formula><mml:math id="M56" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M57" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> in the sample, and <inline-formula><mml:math id="M58" display="inline"><mml:mrow><mml:msub><mml:mi>R</mml:mi><mml:mtext>VPDB</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1.1113</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mn mathvariant="normal">10</mml:mn><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> is the <inline-formula><mml:math id="M59" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow><mml:mo>/</mml:mo><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> ratio of the Vienna Pee Dee Belemnite (VPDB) reference material <xref ref-type="bibr" rid="bib1.bibx26 bib1.bibx15" id="paren.20"/>.</p>
      <p id="d2e1009">Different <inline-formula><mml:math id="M60" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> sources exhibit characteristic <inline-formula><mml:math id="M61" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M62" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M63" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures due to their formation processes. Microbial sources (e.g. wetlands, ruminants) typically emit methane that is strongly depleted in <inline-formula><mml:math id="M64" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>, with values ranging from <inline-formula><mml:math id="M65" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M66" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">55</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx122 bib1.bibx123" id="paren.21"/>. Geographic variability in livestock emissions reflects differences in plant diets, specifically between <inline-formula><mml:math id="M67" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> plants (e.g. wheat, rice, trees) and <inline-formula><mml:math id="M68" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> plants (e.g. maize, sugarcane, tropical grasses), which have distinct carbon isotope compositions <xref ref-type="bibr" rid="bib1.bibx55" id="paren.22"/>. Wetland signatures also vary spatially, with more depleted values observed in boreal regions compared to tropical zones <xref ref-type="bibr" rid="bib1.bibx35 bib1.bibx24 bib1.bibx89" id="paren.23"/>. Fossil fuel-related variability can be large, driven by geological origin and processing techniques, with <inline-formula><mml:math id="M69" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M70" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M71" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures spanning from <inline-formula><mml:math id="M72" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">55</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M73" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">30</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx122 bib1.bibx76" id="paren.24"/>. Geological emissions may also reflect a diversity of geochemical processes, including both thermogenic and microbial pathways, leading to a broader range of <inline-formula><mml:math id="M74" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M75" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M76" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures <xref ref-type="bibr" rid="bib1.bibx122 bib1.bibx27" id="paren.25"/>. Pyrogenic sources (e.g. biomass and biofuel burning) are enriched in <inline-formula><mml:math id="M77" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>, with values ranging from <inline-formula><mml:math id="M78" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">25</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M79" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">15</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx122 bib1.bibx123" id="paren.26"/>, depending on the dominant vegetation type (<inline-formula><mml:math id="M80" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> or <inline-formula><mml:math id="M81" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) <xref ref-type="bibr" rid="bib1.bibx129 bib1.bibx100 bib1.bibx55" id="paren.27"/>. In addition to source-specific isotopic signatures, atmospheric sinks also fractionate methane isotopes through the Kinetic Isotope Effect (KIE). Lighter isotopologues (<inline-formula><mml:math id="M82" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) react faster with major oxidants such as OH, Cl, and <inline-formula><mml:math id="M83" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi><mml:msup><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:msup><mml:mi mathvariant="normal">D</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> than their heavier counterparts (<inline-formula><mml:math id="M84" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>), leading to <inline-formula><mml:math id="M85" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> enrichment in the remaining methane. This process alters the isotopic composition of atmospheric <inline-formula><mml:math id="M86" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal compared to the original source-weighted average signatures.</p>
      <p id="d2e1359">Over the past two decades, a decreasing trend in atmospheric <inline-formula><mml:math id="M87" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M88" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M89" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> has been observed alongside increasing <inline-formula><mml:math id="M90" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> concentrations <xref ref-type="bibr" rid="bib1.bibx87 bib1.bibx75 bib1.bibx116 bib1.bibx117" id="paren.28"/>. This anti-correlation suggests shifts in source contributions, sink processes, or both, providing additional constraints for methane budget reconstructions. Measurements of <inline-formula><mml:math id="M91" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M92" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M93" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> are increasingly integrated into atmospheric inversions to differentiate methane sources through their isotopic signatures <xref ref-type="bibr" rid="bib1.bibx119 bib1.bibx55" id="paren.29"/>. Such data help distinguish co-located or seasonally overlapping sources, assess sectoral contributions, and improve the accuracy of global and regional methane budgets. However, the global network of in situ <inline-formula><mml:math id="M94" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M95" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M96" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> measurements remains sparse, resulting in limited spatial coverage and hampering the characterization of regional isotopic gradients. This motivates the exploration of satellite-based retrievals of isotopic methane, which could substantially enhance global coverage. Feasibility studies using instruments such as GOSAT, TROPOMI, and Sentinel-5/UVNS have demonstrated the potential of remote sensing for <inline-formula><mml:math id="M97" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M98" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M99" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> observations <xref ref-type="bibr" rid="bib1.bibx65 bib1.bibx66" id="paren.30"/>. Recent inversion studies have already begun incorporating <inline-formula><mml:math id="M100" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M101" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M102" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> observations from surface networks <xref ref-type="bibr" rid="bib1.bibx33 bib1.bibx34 bib1.bibx3 bib1.bibx25 bib1.bibx136" id="paren.31"><named-content content-type="pre">e.g.</named-content></xref>, paving the way for future applications that jointly exploit surface and satellite isotopic constraints. However, further studies are needed to properly evaluate possible use of satellite-based isotopic observations in inversions as retrieval uncertainties remain large.</p>
      <p id="d2e1535">A prerequisite for such isotopic inversions is the availability of spatially explicit source signature maps and associated uncertainties. Existing datasets include contributions from <xref ref-type="bibr" rid="bib1.bibx35" id="text.32"/>, <xref ref-type="bibr" rid="bib1.bibx18" id="text.33"/>, <xref ref-type="bibr" rid="bib1.bibx27" id="text.34"/>, <xref ref-type="bibr" rid="bib1.bibx122 bib1.bibx123" id="text.35"/>, <xref ref-type="bibr" rid="bib1.bibx55" id="text.36"/>, <xref ref-type="bibr" rid="bib1.bibx89" id="text.37"/>, and <xref ref-type="bibr" rid="bib1.bibx72" id="text.38"/>. However, limitations remain, particularly in representing uncertainties and covariance structures of isotopic priors <xref ref-type="bibr" rid="bib1.bibx3 bib1.bibx136" id="paren.39"/>. Full sensitivity analyses are also needed to assess the robustness of inversion results with respect to isotopic assumptions <xref ref-type="bibr" rid="bib1.bibx135" id="paren.40"/>.</p>
      <p id="d2e1566">In this study, we present updated spatially explicit <inline-formula><mml:math id="M103" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M104" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M105" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps, with associated uncertainty estimates, to support global and regional methane inversions. Our main objectives are to: <list list-type="custom"><list-item><label>i.</label>
      <p id="d2e1600">improve prior knowledge of isotopic compositions for major <inline-formula><mml:math id="M106" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> sectors and subsectors,</p></list-item><list-item><label>ii.</label>
      <p id="d2e1615">evaluate the influence of the revised maps on modeled atmospheric <inline-formula><mml:math id="M107" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M108" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M109" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> using forward simulations,</p></list-item><list-item><label>iii.</label>
      <p id="d2e1648">quantify the sensitivity of modeled <inline-formula><mml:math id="M110" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M111" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M112" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> to key parameters and regions, and</p></list-item><list-item><label>iv.</label>
      <p id="d2e1681">provide uncertainty estimates and recommendations for integrating isotopic constraints into inversion frameworks.</p></list-item></list></p>
      <p id="d2e1684">Rather than validating the updated source signature maps against atmospheric observations, the sensitivity analysis focuses on quantifying the impact of key sources of uncertainty on modeled atmospheric <inline-formula><mml:math id="M113" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M114" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M115" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> distributions. This sensitivity-centered approach allows us to identify the dominant drivers of variability in the modeled isotopic signal and to provide practical recommendations for future inversion studies. Model-data comparisons, while essential, are beyond the scope of this work and will be addressed in subsequent studies.</p>
      <p id="d2e1716">The structure of the paper is as follows. Section 2 describes the development of the updated <inline-formula><mml:math id="M116" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M117" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M118" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps. Section 3 presents the atmospheric modeling framework used for the sensitivity analysis. Section 4 reports and discusses the main results.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Development of updated <inline-formula><mml:math id="M119" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M120" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M121" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps</title>
      <p id="d2e1786">To improve the spatial and temporal representation of isotopic methane emissions in inverse modeling, we developed a comprehensive set of global maps representing the <inline-formula><mml:math id="M122" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M123" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M124" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures across major methane-emitting sectors and sub-sectors, covering the period 1998–2022. The dataset is available at the ESA Open Science Data portal: (<xref ref-type="bibr" rid="bib1.bibx133" id="altparen.41"/>,  <ext-link xlink:href="https://doi.org/10.57780/ESA-6D202E9" ext-link-type="DOI">10.57780/ESA-6D202E9</ext-link>). These maps have a spatial resolution of <inline-formula><mml:math id="M125" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mi mathvariant="italic">°</mml:mi><mml:mo>×</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mi mathvariant="italic">°</mml:mi></mml:mrow></mml:math></inline-formula> (global coverage) and a monthly time step, providing improved temporal representation and either matching or improving the spatial resolution of previous datasets. It is based on a synthesis of recent gridded data products and regional observations from peer-reviewed literature (Sect. <xref ref-type="sec" rid="Ch1.S2.SS1"/>). The resulting dataset distinguishes five primary source sectors: fossil fuel exploitation and geological (FFG), agriculture and waste (AGW), biomass and biofuel burning (BB), wetlands (WET), and other natural sources (NAT), each composed of multiple underlying sub-sectors detailed (Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>). The associated uncertainties were also calculated (Sect. <xref ref-type="sec" rid="Ch1.S2.SS3"/>). The methodology presented in this section provides a reproducible and publicly available framework to generate <inline-formula><mml:math id="M126" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M127" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M128" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps at global scale, including explicit quantification of associated uncertainties. All acronyms, sector names and dataset abbreviations used throughout this study are summarized in Table S1 in the Supplement for clarity.</p>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Construction of sub-sector isotopic signature maps</title>
      <p id="d2e1884">The construction of these maps relied on the integration of the most up-to-date isotopic datasets available for each methane source sub-sector. Table <xref ref-type="table" rid="T1"/> provides an overview of the aggregated source sectors, their sub-sectors, the associated <inline-formula><mml:math id="M129" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M130" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M131" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> ranges, isotopic data sources, and corresponding emission fluxes. Gridded products were prioritized when available (e.g. <xref ref-type="bibr" rid="bib1.bibx55 bib1.bibx89" id="altparen.42"/>), and were supplemented by regional datasets (e.g. <xref ref-type="bibr" rid="bib1.bibx74" id="altparen.43"/>) or literature-based estimates when spatially explicit data were lacking. To ensure representativeness at the global scale, a combination of pixel-level (P), regional (R), and global (G) datasets was used. The temporal resolution of the isotopic signatures was preserved when available in the source datasets, using annual (A) or monthly (M) variations. Otherwise, constant (C) values over the 1998–2022 period were assumed. Each entry in Table <xref ref-type="table" rid="T1"/> is associated with metadata indicating its spatial (P, R, G) and temporal (C, A, M) resolution. All isotopic signatures are expressed relative to the VPDB standard; a discussion of the VPDB vs. historical PDB reference scales and their negligible impact on the simulations is provided in Sect. S1.1 in the Supplement. The following sections detail the specific methodologies applied to key source categories and describe how temporal or spatial gaps were addressed to produce a consistent, gridded isotopic dataset.</p>

<table-wrap id="T1" specific-use="star"><label>Table 1</label><caption><p id="d2e1930">Methane emission sectors aggregated for atmospheric modeling, including representative <inline-formula><mml:math id="M132" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M133" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M134" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> isotopic signatures and flux estimates over 1998–2022. For each major sector (FFG, AGW, BB, WET, NAT), sub-sectoral values are compiled and aggregated using flux-weighted averages. Isotopic signature ranges reflect observed variability within each sub-sector, based on available spatial and temporal resolution: (P) pixel-level, (R) regional, or (G) global data, and (C) constant, (A) annual, or (M) monthly data. Flux estimates are derived from the Emissions Database for Global Atmospheric Research (EDGARv8; <xref ref-type="bibr" rid="bib1.bibx23" id="altparen.44"/>), the Global Fire Emissions Database (GFED4s; <xref ref-type="bibr" rid="bib1.bibx143" id="altparen.45"/>), and the Global Methane Budget (GMB; <xref ref-type="bibr" rid="bib1.bibx68" id="altparen.46"/>). Bold font is used in the “Aggregated” rows to mark the flux-weighted sector-level values (both the aggregated δ<sup>13</sup>C-CH<sub>4</sub> source signature and the aggregated flux).</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="6">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Sectors</oasis:entry>
         <oasis:entry colname="col2">Sub-sectors</oasis:entry>
         <oasis:entry colname="col3">Source Signature (<inline-formula><mml:math id="M137" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>, [min–max])</oasis:entry>
         <oasis:entry colname="col4">Isotopic Signature References</oasis:entry>
         <oasis:entry colname="col5">Flux (<inline-formula><mml:math id="M138" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, [min–max])</oasis:entry>
         <oasis:entry colname="col6">Flux References</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">FFG</oasis:entry>
         <oasis:entry colname="col2">Coal</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M139" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>43.7 (<inline-formula><mml:math id="M140" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>64.1 to <inline-formula><mml:math id="M141" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>30.8]</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx55 bib1.bibx74" id="text.47"><named-content content-type="post">R,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">35.6 [23.4–46.8]</oasis:entry>
         <oasis:entry colname="col6">EDGARv8</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Oil and gas</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M142" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>44.0 (<inline-formula><mml:math id="M143" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>65.0 to <inline-formula><mml:math id="M144" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>29.1]</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx55 bib1.bibx74" id="text.48"><named-content content-type="post">R,A</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">73.2 [63.0–81.5]</oasis:entry>
         <oasis:entry colname="col6">EDGARv8</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Geological</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M145" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>46.6 (<inline-formula><mml:math id="M146" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>68.0 to <inline-formula><mml:math id="M147" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>24.3]</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx27" id="text.49"><named-content content-type="post">P,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">21.1</oasis:entry>
         <oasis:entry colname="col6">GMB</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Aggregated</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M148" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>44.2 [<inline-formula><mml:math id="M149" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>65.0 to <inline-formula><mml:math id="M150" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>24.3]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"><bold>129.9</bold></oasis:entry>
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">AGW</oasis:entry>
         <oasis:entry colname="col2">Livestock</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M151" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>65.8 (<inline-formula><mml:math id="M152" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>67.8 to <inline-formula><mml:math id="M153" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>54.6]</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx55" id="text.50"><named-content content-type="post">P,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">101.4 [91.0–112.3]</oasis:entry>
         <oasis:entry colname="col6">EDGARv8</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Wastewater</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M154" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>50.9</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx74" id="text.51"><named-content content-type="post">G,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">38.4 [30.4–46.8]</oasis:entry>
         <oasis:entry colname="col6">EDGARv8</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Landfills</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M155" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>56.2</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx74" id="text.52"><named-content content-type="post">G,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">33.6 [30.4–40.2]</oasis:entry>
         <oasis:entry colname="col6">EDGARv8</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Agricultural waste</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M156" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>54.9</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx74" id="text.53"><named-content content-type="post">G,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">11.7 [10.8–12.7]</oasis:entry>
         <oasis:entry colname="col6">EDGARv8</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Rice</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M157" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>59.9</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx74" id="text.54"><named-content content-type="post">G,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">35.8 [32.7–37.4]</oasis:entry>
         <oasis:entry colname="col6">EDGARv8</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Aggregated</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M158" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>60.2 [<inline-formula><mml:math id="M159" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>67.6 to <inline-formula><mml:math id="M160" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>50.9]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"><bold>221.0</bold></oasis:entry>
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">BB</oasis:entry>
         <oasis:entry colname="col2">Biofuel burning</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M161" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>24.3 (<inline-formula><mml:math id="M162" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>26.7 to <inline-formula><mml:math id="M163" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>12.6]</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx55" id="text.55"><named-content content-type="post">P,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">11.9 [11.2–12.3]</oasis:entry>
         <oasis:entry colname="col6">EDGARv8</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Biomass burning</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M164" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>24.2 (<inline-formula><mml:math id="M165" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>26.7 to <inline-formula><mml:math id="M166" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>12.6]</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx55" id="text.56"><named-content content-type="post">P,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">13.2 [9.3–20.2]</oasis:entry>
         <oasis:entry colname="col6">GFED4s</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Aggregated</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M167" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>24.3 [<inline-formula><mml:math id="M168" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>26.7 to <inline-formula><mml:math id="M169" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>12.6]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"><bold>25.1</bold></oasis:entry>
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">WET</oasis:entry>
         <oasis:entry colname="col2">Wetlands</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M170" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>58.6 (<inline-formula><mml:math id="M171" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>73.6 to <inline-formula><mml:math id="M172" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>18.2]</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx89" id="text.57"><named-content content-type="post">P,M</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">151.6</oasis:entry>
         <oasis:entry colname="col6">GMB</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Aggregated</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M173" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>58.6 [<inline-formula><mml:math id="M174" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>73.6 to <inline-formula><mml:math id="M175" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>18.2]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"><bold>151.6</bold></oasis:entry>
         <oasis:entry colname="col6"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">NAT</oasis:entry>
         <oasis:entry colname="col2">Termites</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M176" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>63.4</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx137" id="text.58"><named-content content-type="post">G,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">9.9</oasis:entry>
         <oasis:entry colname="col6">GMB</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Oceans</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M177" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>42.0</oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx106" id="text.59"><named-content content-type="post">G,C</named-content></xref>
                      
                    </oasis:entry>
         <oasis:entry colname="col5">11.5</oasis:entry>
         <oasis:entry colname="col6">GMB</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Aggregated</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M178" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>51.9 [<inline-formula><mml:math id="M179" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>63.4 to <inline-formula><mml:math id="M180" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>42.0]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"><bold>21.5</bold></oasis:entry>
         <oasis:entry colname="col6"/>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

<sec id="Ch1.S2.SS1.SSS1">
  <label>2.1.1</label><title>Treatment of European fossil fuel isotopic signatures</title>
      <p id="d2e2808">For fossil fuel emissions in Europe, regional measurements from the European Methane Isotope Database (EMID; <xref ref-type="bibr" rid="bib1.bibx74" id="altparen.60"/>) were combined with the global inventory from <xref ref-type="bibr" rid="bib1.bibx55" id="text.61"/> to improve the spatial accuracy of isotopic signatures. The <xref ref-type="bibr" rid="bib1.bibx55" id="text.62"/> dataset, based on the compilation by <xref ref-type="bibr" rid="bib1.bibx123" id="text.63"/>, includes isotopic data from over 13 000 locations from 347 references, though it remains largely U.S. centered. The EMID database provides additional coverage, including both literature data and new measurements from the MEMO<sup>2</sup> project for fossil fuel sources over Europe <xref ref-type="bibr" rid="bib1.bibx28" id="paren.64"/>. The extended global database, combining EMID with <xref ref-type="bibr" rid="bib1.bibx123" id="text.65"/> and MEMO<sup>2</sup>, consists of over 13 313 <inline-formula><mml:math id="M183" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M184" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> measurements from 64 countries.</p>
      <p id="d2e2866">The integration of these two datasets was conducted as follows: <list list-type="order"><list-item>
      <p id="d2e2871">Country-level average <inline-formula><mml:math id="M185" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M186" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M187" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures were computed from EMID for some European countries (e.g. UK, Germany, Poland, Romania, France), corresponding to those for which data are available in the EMID inventory.</p></list-item><list-item>
      <p id="d2e2904">These averages were then combined with <xref ref-type="bibr" rid="bib1.bibx55" id="text.66"/> data using a weighting factor that accounts for the number of additional observations in EMID compared to <xref ref-type="bibr" rid="bib1.bibx123" id="text.67"/> dataset.</p></list-item></list> The resulting aggregated values are presented in Table S2 in the Supplement.</p>
</sec>
<sec id="Ch1.S2.SS1.SSS2">
  <label>2.1.2</label><title>Temporal extrapolation</title>
      <p id="d2e2923">To ensure full temporal coverage over the 1998–2022 period, extrapolation was required for certain datasets whose original time series ended prematurely, specifically for the oil and gas and wetland sub-sectors. In both cases, specific strategies were applied based on known emission trends and isotopic characteristics of source signatures.</p>
      <p id="d2e2926">For the oil and gas sub-sector, the dataset from <xref ref-type="bibr" rid="bib1.bibx55" id="text.68"/> ends in 2016. Post-2016 values were extrapolated only for U.S. data, based on documented trends in U.S. unconventional gas production (U.S. Energy Information Administration, EIA, <uri>https://www.eia.gov/energyexplained/us-energy-facts</uri>, last access: 14 March 2025), notably shale gas, which typically exhibits lighter <inline-formula><mml:math id="M188" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M189" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M190" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures than conventional sources <xref ref-type="bibr" rid="bib1.bibx122" id="paren.69"/>. Basin-level variability in both gas production and isotopic composition was accounted for using data from the EIA natural gas reports (<uri>https://www.eia.gov/naturalgas/weekly/</uri>, last access: 9 March 2025) and published isotopic measurements <xref ref-type="bibr" rid="bib1.bibx78" id="paren.70"/>. Outside the U.S., signatures values were held constant. We adopted a two-step method to extrapolate U.S. <inline-formula><mml:math id="M191" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M192" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M193" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values post-2016: <list list-type="order"><list-item>
      <p id="d2e3005">computing basin-weighted <inline-formula><mml:math id="M194" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M195" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M196" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values based on production volumes, using shale gas data per basin  (EIA, <uri>https://www.eia.gov/dnav/ng/ng_prod_shalegas_s1_a.html</uri>, last access: 9 March 2025) and basin-specific isotopic signatures <xref ref-type="bibr" rid="bib1.bibx78" id="paren.71"/>;</p></list-item><list-item>
      <p id="d2e3044">adjusting national-scale <inline-formula><mml:math id="M197" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M198" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M199" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values according to the evolving share of shale gas in total production  (EIA, <uri>https://www.eia.gov/naturalgas/weekly/</uri>, last access: 9 March 2025).</p></list-item></list></p>
      <p id="d2e3079">For wetlands, the monthly <inline-formula><mml:math id="M200" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M201" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M202" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps from <xref ref-type="bibr" rid="bib1.bibx89" id="text.72"/> also end in 2016. To extend the dataset beyond this point, we extrapolated the 2016 seasonal cycle linearly and incorporated the long-term trend in source signatures of <inline-formula><mml:math id="M203" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:mrow></mml:math></inline-formula> observed over the 1984–2016 period <xref ref-type="bibr" rid="bib1.bibx89" id="paren.73"/>.</p>
</sec>
</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>Aggregation into source sectors</title>
      <p id="d2e3149">To facilitate the integration of <inline-formula><mml:math id="M204" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M205" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M206" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures into atmospheric modeling and to optimize computational efficiency, detailed source sub-sectors were aggregated into broader emission sectors using flux-weighted mean values (more details in Sect. S1.2 in the Supplement). This aggregation preserves the key isotopic characteristics of different emission types while reducing model complexity. The classification follows the methodology adopted in the Global Methane Budget <xref ref-type="bibr" rid="bib1.bibx111" id="paren.74"><named-content content-type="pre">GMB</named-content></xref>, grouping methane emissions into five principal source categories (Table <xref ref-type="table" rid="T1"/>): <list list-type="bullet"><list-item>
      <p id="d2e3190">FFG includes emissions from oil, gas, coal, industrial activities, transport, and natural geological seepage.</p></list-item><list-item>
      <p id="d2e3194">AGW encompasses emissions from enteric fermentation, rice cultivation, manure management, and waste decomposition.</p></list-item><list-item>
      <p id="d2e3198">BB sector comprises emissions from open biomass combustion and biofuel use.</p></list-item><list-item>
      <p id="d2e3202">WET includes natural wetland emissions as well as emissions from freshwater systems such as lakes, ponds, reservoirs, rivers, and streams.</p></list-item><list-item>
      <p id="d2e3206">NAT sector covers natural non-wetland emissions, including mostly those from termites and oceanic sources.</p></list-item></list></p>
      <p id="d2e3209">This aggregation aims to ensure isotopic representativity within each sector, in line with recent recommendations for source signature consistency <xref ref-type="bibr" rid="bib1.bibx67" id="paren.75"/>. An exception may apply to the NAT sector, which encompasses heterogeneous processes (e.g. termite emissions vs. oceanic sources) that are not co-located. These sub-sources were grouped primarily due to their relatively small fluxes and to limit the number of categories for computational efficiency, rather than based on isotopic or spatial consistency. A comprehensive mapping between detailed subcategories and the aggregated sectors used in this study is provided in Table <xref ref-type="table" rid="T1"/>. In cases where isotopic data were missing for a specific pixel, flux-weighted average values were used so that each sector's data covered the entire domain.</p>
      <p id="d2e3217">Both the aggregated maps for the five main source sectors and the underlying maps for the 14 sub-sectors listed in Table <xref ref-type="table" rid="T1"/> are publicly distributed (see Code and data availability). This dual format allows users to either directly use the inversion-ready aggregated product, or to re-aggregate the sub-sector maps using their own flux-weighting scheme, sectoral classification, or extended sub-sector breakdown if their inversion framework requires a finer or different grouping.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <label>2.3</label><title>Uncertainty assessment of aggregated source signatures</title>
      <p id="d2e3231">This section describes how uncertainties in aggregated <inline-formula><mml:math id="M207" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M208" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M209" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures are estimated. All uncertainties are evaluated at the global scale, i.e. they are not spatially resolved at the grid-cell level. The overall propagation pathway, from sub-sector measurements to inversion error structures, is summarized schematically in Fig. <xref ref-type="fig" rid="F1"/>. In what follows, we describe the three components of this propagation chain: the total uncertainty <inline-formula><mml:math id="M210" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> combining all contributions (Sect. <xref ref-type="sec" rid="Ch1.S2.SS3.SSS1"/>), the propagated uncertainty <inline-formula><mml:math id="M211" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> derived from sub-sector variability (Sect. <xref ref-type="sec" rid="Ch1.S2.SS3.SSS2"/>), and the aggregation uncertainty <inline-formula><mml:math id="M212" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> reflecting inventory choices (Sect. <xref ref-type="sec" rid="Ch1.S2.SS3.SSS3"/>).</p>

      <fig id="F1" specific-use="star"><label>Figure 1</label><caption><p id="d2e3307">Schematic overview of the uncertainty propagation pathway for <inline-formula><mml:math id="M213" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M214" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M215" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures. Sub-sector isotopic uncertainties (<inline-formula><mml:math id="M216" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>), derived from Monte Carlo simulations (lower bound) and literature standard deviations (upper bound), are propagated to the sector level (<inline-formula><mml:math id="M217" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) via flux-weighted error propagation (Eq. 4). The aggregation uncertainty (<inline-formula><mml:math id="M218" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>), estimated from sensitivity tests using different emission inventories (Eq. 5), is combined with <inline-formula><mml:math id="M219" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> to yield the total sectoral uncertainty (<inline-formula><mml:math id="M220" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, Eq. 2). In atmospheric inversion frameworks, <inline-formula><mml:math id="M221" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> informs either the prior error covariance matrix (<inline-formula><mml:math id="M222" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula>) if isotopic source signatures are optimized, or the observation error covariance matrix (<inline-formula><mml:math id="M223" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula>) if they are held fixed (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>).</p></caption>
          <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f01.png"/>

        </fig>


<sec id="Ch1.S2.SS3.SSS1">
  <label>2.3.1</label><title>Total uncertainty (<inline-formula><mml:math id="M224" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>)</title>
      <p id="d2e3450">To quantify the uncertainty associated with the aggregated <inline-formula><mml:math id="M225" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M226" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M227" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures (<inline-formula><mml:math id="M228" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>), we consider two main components: (i) the propagated uncertainty from sub-sector level to sector level (<inline-formula><mml:math id="M229" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>), i.e. the intrinsic isotopic uncertainty from sub-sector, and (ii) the aggregation uncertainties (<inline-formula><mml:math id="M230" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>), i.e. the variability introduced when aggregating sub-sector signatures into sector-level values, using a given set of flux weights from prior inventories. Assuming that the two types of uncertainties are independent, the total uncertainty for each aggregated sector is calculated by combining these two components:

                  <disp-formula id="Ch1.E2" content-type="numbered"><label>2</label><mml:math id="M231" display="block"><mml:mstyle class="stylechange" displaystyle="true"/><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:msqrt><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:msqrt></mml:mrow></mml:math></disp-formula></p>
      <p id="d2e3548">The corresponding relative uncertainty (in percentage) is then calculated as:

                  <disp-formula id="Ch1.E3" content-type="numbered"><label>3</label><mml:math id="M232" display="block"><mml:mstyle displaystyle="true" class="stylechange"/><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mtext>Relative uncertainty (%)</mml:mtext><mml:mo>=</mml:mo><mml:mfenced close=")" open="("><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow><mml:mrow><mml:mfenced open="|" close="|"><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi mathvariant="italic">δ</mml:mi><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mtext>sector</mml:mtext></mml:msub></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:mfenced></mml:mrow></mml:mfrac></mml:mstyle></mml:mfenced><mml:mo>×</mml:mo><mml:mn mathvariant="normal">100</mml:mn></mml:mrow></mml:math></disp-formula>

            where <inline-formula><mml:math id="M233" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> corresponds to the propagated uncertainty at the sector level derived from sub-sector uncertainties (<inline-formula><mml:math id="M234" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), <inline-formula><mml:math id="M235" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> represents the uncertainty associated with the aggregation method, estimated from sensitivity tests (<inline-formula><mml:math id="M236" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) and <inline-formula><mml:math id="M237" display="inline"><mml:mover accent="true"><mml:mrow><mml:msup><mml:mi mathvariant="italic">δ</mml:mi><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mtext>sector</mml:mtext></mml:msub></mml:mrow><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:math></inline-formula> denotes the mean isotopic signature of the aggregated sector (<inline-formula><mml:math id="M238" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>).</p>
      <p id="d2e3658">Because the propagated uncertainty <inline-formula><mml:math id="M239" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is provided as a range, the resulting total uncertainty <inline-formula><mml:math id="M240" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is also expressed as a corresponding range rather than a single value.</p>
</sec>
<sec id="Ch1.S2.SS3.SSS2">
  <label>2.3.2</label><title>Propagated uncertainty from sub-sectors (<inline-formula><mml:math id="M241" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>)</title>
      <p id="d2e3703">The term <inline-formula><mml:math id="M242" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> represents the propagated uncertainty from sub-sector isotopic composition (<inline-formula><mml:math id="M243" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) to the aggregated sector level. First, the isotopic uncertainty for each sub-sector (<inline-formula><mml:math id="M244" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) is estimated using two complementary approaches, depending on the origin of the data: <list list-type="bullet"><list-item>
      <p id="d2e3741">The standard deviations of <inline-formula><mml:math id="M245" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M246" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M247" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values reported in the literature, using the dataset compiled by <xref ref-type="bibr" rid="bib1.bibx73" id="text.76"/>, which captures spatial variability and methodological dispersion;</p></list-item><list-item>
      <p id="d2e3777">The uncertainty values reported by <xref ref-type="bibr" rid="bib1.bibx55" id="text.77"/>, who derived them from 10 000 Monte Carlo simulations at the grid-cell level, explicitly propagating measurement and modeling errors through source attribution and mixing processes.</p></list-item></list></p>
      <p id="d2e3783">The Monte Carlo approach provides a precise uncertainty estimate directly linked to sub-sector diversity but may underestimate broader, large-scale variability and inter-regional differences. Conversely, the literature-based standard deviation offers a more conservative benchmark that captures additional inter-study, regional, and methodological variability. The two approaches (literature-based standard deviations and Monte Carlo uncertainties) provide lower and upper estimates of the sub-sector isotopic uncertainty.</p>
      <p id="d2e3786">Second, the sub-sector uncertainties (<inline-formula><mml:math id="M248" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) are propagated into the aggregated sector uncertainty component (<inline-formula><mml:math id="M249" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) using a flux-weighted error propagation approach:

                  <disp-formula id="Ch1.E4" content-type="numbered"><label>4</label><mml:math id="M250" display="block"><mml:mstyle displaystyle="true" class="stylechange"/><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:msqrt><mml:mrow><mml:munder><mml:mo movablelimits="false">∑</mml:mo><mml:mi>i</mml:mi></mml:munder><mml:msup><mml:mfenced close=")" open="("><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:mfrac></mml:mstyle></mml:mfenced><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:msqrt></mml:mrow></mml:math></disp-formula>

            where <inline-formula><mml:math id="M251" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the flux of sub-sector <inline-formula><mml:math id="M252" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> (Tg <inline-formula><mml:math id="M253" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>), <inline-formula><mml:math id="M254" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is the total flux of the aggregated sector (Tg <inline-formula><mml:math id="M255" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>), and <inline-formula><mml:math id="M256" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the isotopic uncertainty of sub-sector <inline-formula><mml:math id="M257" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> (<inline-formula><mml:math id="M258" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>).</p>
      <p id="d2e3943">The aggregated sector uncertainty (<inline-formula><mml:math id="M259" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) is reported as a range, with the lower bound corresponding to the Monte Carlo estimate and the upper bound corresponding to the literature-based estimate.</p>
</sec>
<sec id="Ch1.S2.SS3.SSS3">
  <label>2.3.3</label><title>Aggregation uncertainty (<inline-formula><mml:math id="M260" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>)</title>
      <p id="d2e3977">This component reflects the sensitivity of aggregated signatures to methodological choices of weighting fluxes in the construction of the aggregated sector dataset. It is evaluated through a series of sensitivity tests (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS2"/>), and computed as the standard deviation across the resulting aggregation scenarios:

                  <disp-formula id="Ch1.E5" content-type="numbered"><label>5</label><mml:math id="M261" display="block"><mml:mstyle displaystyle="true" class="stylechange"/><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:msqrt><mml:mrow><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mi>N</mml:mi></mml:mfrac></mml:mstyle><mml:munderover><mml:mo movablelimits="false">∑</mml:mo><mml:mrow><mml:mi>j</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mi>N</mml:mi></mml:munderover><mml:mo>(</mml:mo><mml:msub><mml:mover accent="true"><mml:mi>x</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover><mml:mi>j</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:mover accent="true"><mml:mi>x</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover><mml:msup><mml:mo>)</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:msqrt></mml:mrow></mml:math></disp-formula>

            where <inline-formula><mml:math id="M262" display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mi>x</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover><mml:mi>j</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the mean isotopic signature derived from aggregation method <inline-formula><mml:math id="M263" display="inline"><mml:mi>j</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M264" display="inline"><mml:mover accent="true"><mml:mi>x</mml:mi><mml:mo mathvariant="normal">¯</mml:mo></mml:mover></mml:math></inline-formula> is the overall mean isotopic signature across all tested methods, and <inline-formula><mml:math id="M265" display="inline"><mml:mi>N</mml:mi></mml:math></inline-formula> is the number of tested aggregation methods.</p>
      <p id="d2e4078">In summary, this framework provides consistent tools to estimate sectoral <inline-formula><mml:math id="M266" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M267" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M268" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> uncertainties, combining sub-sector variability and aggregation effects. Beyond sectoral aggregation, isotopic uncertainties also carry a latitudinal dimension, driven notably by the distribution of <inline-formula><mml:math id="M269" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M270" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> plants across source sectors and by stratospheric transport processes; these spatial gradients are discussed further in Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS1"/>. Because uncertainties in isotopic signature values and their spatial allocation propagate into regional and global inversions, ultimately influencing source attribution, it is particularly important to assess them. The resulting uncertainties are directly usable in atmospheric models and inversions to inform prior error structures and guide optimization choices (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>).</p>
</sec>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Atmospheric framework for sensitivity analysis</title>
      <p id="d2e4147">Building on recent flux inventories and isotopic signature datasets, we developed updated <inline-formula><mml:math id="M271" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M272" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M273" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps suitable for atmospheric modeling and inversion studies (see Sect. <xref ref-type="sec" rid="Ch1.S2"/>). This section presents how these maps are integrated into forward atmospheric simulations to assess how key parameters uncertainties propagate to the modeled <inline-formula><mml:math id="M274" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M275" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M276" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal. We first describe the modeling framework used for the simulations (Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>), then detail the sensitivity experiments designed to explore the influence of critical drivers, including methane fluxes, fluxes used for isotopic aggregation, OH fields, OH kinetic isotope effects, and isotopic source signatures (Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>).</p>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Description of atmospheric simulations</title>
      <p id="d2e4222">To assess the influence of key parameters and evaluate the impact of the updated <inline-formula><mml:math id="M277" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M278" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M279" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signature dataset, we conducted a sensitivity analysis based on forward simulations of methane mole fractions and <inline-formula><mml:math id="M280" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M281" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M282" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signals over the period 1998–2022. These simulations were performed within the Community Inversion Framework (CIF; <xref ref-type="bibr" rid="bib1.bibx5" id="altparen.78"/>). The CIF was extended by <xref ref-type="bibr" rid="bib1.bibx134" id="text.79"/> to incorporate isotopic constraints, enabling the joint simulation and assimilation of <inline-formula><mml:math id="M283" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions and their <inline-formula><mml:math id="M284" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M285" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M286" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> composition. The following subsections describe in detail all components of the forward simulations.</p>
<sec id="Ch1.S3.SS1.SSS1">
  <label>3.1.1</label><title>Global transport model</title>
      <p id="d2e4337">The simulations were conducted using the LMDz transport model, a component of the coupled model from the Institut Pierre-Simon Laplace (IPSL-CM), developed at the Laboratoire de Météorologie Dynamique (LMD; <xref ref-type="bibr" rid="bib1.bibx45" id="altparen.80"/>). The offline version was used, driven by ECMWF ERA-Interim reanalyses, as described in <xref ref-type="bibr" rid="bib1.bibx20" id="text.81"/>. LMDz operates at a horizontal resolution of <inline-formula><mml:math id="M287" display="inline"><mml:mrow><mml:mn mathvariant="normal">3.75</mml:mn><mml:mi mathvariant="italic">°</mml:mi><mml:mo>×</mml:mo><mml:mn mathvariant="normal">1.875</mml:mn><mml:mi mathvariant="italic">°</mml:mi></mml:mrow></mml:math></inline-formula>, with 39 vertical hybrid sigma-pressure levels extending up to approximately 75 <inline-formula><mml:math id="M288" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula>. The model time step is 30 <inline-formula><mml:math id="M289" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">min</mml:mi></mml:mrow></mml:math></inline-formula>. Vertical diffusion is parameterized following the local approach of <xref ref-type="bibr" rid="bib1.bibx64" id="text.82"/>, while deep convection is represented using the Kerry Emanuel scheme <xref ref-type="bibr" rid="bib1.bibx101" id="paren.83"/>.</p>
</sec>
<sec id="Ch1.S3.SS1.SSS2">
  <label>3.1.2</label><title>Emissions fluxes</title>
      <p id="d2e4393">Source categories are described in Table <xref ref-type="table" rid="T1"/> with the following emission fluxes: All flux datasets were selected to ensure consistency with the Global Methane Budget (GMB) framework <xref ref-type="bibr" rid="bib1.bibx110 bib1.bibx111" id="paren.84"/>, which provides the reference basis for methane emission assessments. <list list-type="bullet"><list-item>
      <p id="d2e4403"><italic>Anthropogenic sources.</italic> Emissions from agriculture, waste, fossil fuel exploitation, and biofuel combustion are taken from the EDGARv8 inventory <xref ref-type="bibr" rid="bib1.bibx23" id="paren.85"/>. This dataset provides detailed activity data and region-specific emission factors, enabling realistic representation of spatial and temporal variability across sectors and regions.</p></list-item><list-item>
      <p id="d2e4412"><italic>Biomass burning.</italic> Emissions from wildfires and agricultural burning are derived from the Global Fire Emissions Database (GFED4s) <xref ref-type="bibr" rid="bib1.bibx143" id="paren.86"/>. GFED4s integrates satellite observations of burned area, fire radiative power, and biogeochemical model outputs to provide monthly <inline-formula><mml:math id="M290" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> flux estimates.</p></list-item><list-item>
      <p id="d2e4432"><italic>Wetlands.</italic> Wetland emissions are estimated using the multi-model mean of 11 process-based models compiled within the Global Methane Budget framework <xref ref-type="bibr" rid="bib1.bibx68" id="paren.87"/>. These fluxes are provided as monthly climatological values.</p></list-item><list-item>
      <p id="d2e4441"><italic>Freshwater systems.</italic> Emissions from lakes and reservoirs are based on the <inline-formula><mml:math id="M291" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> flux maps by <xref ref-type="bibr" rid="bib1.bibx127" id="text.88"/>. Initial global emissions are estimated at 95 <inline-formula><mml:math id="M292" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, reduced to 73 <inline-formula><mml:math id="M293" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> after ice-cover corrections. Following <xref ref-type="bibr" rid="bib1.bibx68" id="text.89"/>, emissions are further rescaled by a factor of one-third, resulting in a global total of 53 <inline-formula><mml:math id="M294" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx111" id="paren.90"/>. We acknowledge that freshwater flux estimates remain subject to large uncertainties, arising from poorly mapped inland water extent, complex emission pathways, and spatial variability in methanotrophy <xref ref-type="bibr" rid="bib1.bibx141 bib1.bibx59 bib1.bibx120" id="paren.91"><named-content content-type="pre">e.g.</named-content></xref>. These uncertainties are further discussed in Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS2"/>.</p></list-item><list-item>
      <p id="d2e4526"><italic>Termites.</italic> Termite emissions follow <xref ref-type="bibr" rid="bib1.bibx68" id="text.92"/> based on the S. Castaldi model, providing a spatially explicit global climatology without accounting for seasonal variability.</p></list-item><list-item>
      <p id="d2e4535"><italic>Geological methane.</italic> Geological emissions use the gridded climatology from <xref ref-type="bibr" rid="bib1.bibx27" id="text.93"/>, rescaled to a total global flux of 21 <inline-formula><mml:math id="M295" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> by <xref ref-type="bibr" rid="bib1.bibx68" id="text.94"/>. Offshore geological emissions, including marine seepage, are excluded to avoid double counting. We note that geological emission estimates remain uncertain; ice core-based constraints suggest that pre-industrial geological emissions may have been substantially lower <xref ref-type="bibr" rid="bib1.bibx95" id="paren.95"/>, though the current value follows the Global Methane Budget framework <xref ref-type="bibr" rid="bib1.bibx68" id="paren.96"/> for consistency with the broader modeling setup.</p></list-item><list-item>
      <p id="d2e4576"><italic>Oceanic methane.</italic> Ocean emissions rely on the climatological dataset of <xref ref-type="bibr" rid="bib1.bibx147" id="text.97"/>, which combines microbial <inline-formula><mml:math id="M296" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> production in the water column and geological seepage from seafloor sediments. These emissions are considered seasonally invariant and included as a static component of the total <inline-formula><mml:math id="M297" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> flux budget <xref ref-type="bibr" rid="bib1.bibx68" id="paren.98"/>.</p></list-item></list></p>
</sec>
<sec id="Ch1.S3.SS1.SSS3">
  <label>3.1.3</label><title>Initial conditions</title>
      <p id="d2e4617">Initial conditions for <inline-formula><mml:math id="M298" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M299" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M300" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M301" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> for the year 1998 were derived from an inversion covering the period 1988–2020 <xref ref-type="bibr" rid="bib1.bibx136" id="paren.99"/>. A spin-up period from 1998 to 2016 was used to allow the model to adjust to realistic atmospheric gradients, particularly for <inline-formula><mml:math id="M302" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M303" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M304" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx132" id="paren.100"/>. Only the period 2016–2020 is analyzed to ensure that the model has reached a stable state and to enable direct comparison between simulations, which differ only from the perturbed parameters (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>).</p>
</sec>
<sec id="Ch1.S3.SS1.SSS4">
  <label>3.1.4</label><title>Chemistry</title>
      <p id="d2e4707">Methane oxidation is simulated using the generic chemical module of the offline LMDz model <xref ref-type="bibr" rid="bib1.bibx96 bib1.bibx135" id="paren.101"/>. The chemical scheme includes reactions with hydroxyl radicals (OH), excited atomic oxygen (<inline-formula><mml:math id="M305" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi><mml:msup><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:msup><mml:mi mathvariant="normal">D</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>), and chlorine radicals (Cl). Oxidant concentrations are prescribed from precomputed daily 3-D fields summarized in Table <xref ref-type="table" rid="T2"/>. <list list-type="bullet"><list-item>
      <p id="d2e4734"><italic>Hydroxyl radicals (OH).</italic> OH is the primary sink for atmospheric methane. Monthly mean OH fields are taken from LMDz-INCA simulations <xref ref-type="bibr" rid="bib1.bibx41" id="paren.102"/>, driven by consistent meteorological forcing with the transport model.</p></list-item><list-item>
      <p id="d2e4743"><italic>Excited atomic oxygen (O</italic>(<sup>1</sup><italic>D</italic>). <inline-formula><mml:math id="M307" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi><mml:msup><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:msup><mml:mi mathvariant="normal">D</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> contributes mainly to methane oxidation in the stratosphere. A monthly climatology from the TRANSCOM project <xref ref-type="bibr" rid="bib1.bibx92" id="paren.103"/> is used.</p></list-item><list-item>
      <p id="d2e4780"><italic>Chlorine radicals (Cl).</italic> Methane destruction by Cl radicals is particularly relevant in both the marine boundary layer and the stratosphere. Cl fields are based on the dataset of <xref ref-type="bibr" rid="bib1.bibx145" id="text.104"/>, as recommended by <xref ref-type="bibr" rid="bib1.bibx135" id="text.105"/>, and include both tropospheric and stratospheric concentrations.</p></list-item></list></p>

<table-wrap id="T2" specific-use="star"><label>Table 2</label><caption><p id="d2e4794">Fractionation coefficients for methane oxidation reactions with OH, <inline-formula><mml:math id="M308" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi><mml:mo>(</mml:mo><mml:msup><mml:mi/><mml:mn mathvariant="normal">1</mml:mn></mml:msup><mml:mi mathvariant="normal">D</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, and Cl. The kinetic isotope effect (KIE) values are shown for each reaction, along with their respective references and sources of the 3D oxidant fields. For Cl, the KIE is expressed as a temperature-dependent exponential function, where <inline-formula><mml:math id="M309" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> denotes temperature in Kelvin (<inline-formula><mml:math id="M310" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi></mml:mrow></mml:math></inline-formula>).</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="4">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Oxidant</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M311" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>(</mml:mo><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow><mml:mo>)</mml:mo><mml:mo>/</mml:mo><mml:mi>k</mml:mi><mml:mo>(</mml:mo><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">Reference</oasis:entry>
         <oasis:entry colname="col4">3D Field Source</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">OH</oasis:entry>
         <oasis:entry colname="col2">1.0039</oasis:entry>
         <oasis:entry colname="col3">
                      <xref ref-type="bibr" rid="bib1.bibx108" id="text.106"/>
                    </oasis:entry>
         <oasis:entry colname="col4">LMDz-INCA <xref ref-type="bibr" rid="bib1.bibx41" id="paren.107"/></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M312" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">O</mml:mi><mml:msup><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:msup><mml:mi mathvariant="normal">D</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">1.013</oasis:entry>
         <oasis:entry colname="col3">
                      <xref ref-type="bibr" rid="bib1.bibx108" id="text.108"/>
                    </oasis:entry>
         <oasis:entry colname="col4">TRANSCOM <xref ref-type="bibr" rid="bib1.bibx92" id="paren.109"/></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Cl</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M313" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.043</mml:mn><mml:mo>×</mml:mo><mml:msup><mml:mi mathvariant="normal">e</mml:mi><mml:mrow><mml:mn mathvariant="normal">6.455</mml:mn><mml:mi>K</mml:mi><mml:mo>/</mml:mo><mml:mi>T</mml:mi></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">
                      <xref ref-type="bibr" rid="bib1.bibx107" id="text.110"/>
                    </oasis:entry>
         <oasis:entry colname="col4">
                      <xref ref-type="bibr" rid="bib1.bibx145" id="text.111"/>
                    </oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d2e4999">Isotopic fractionation from <inline-formula><mml:math id="M314" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> oxidation is expressed by the kinetic isotope effects (KIEs), which quantify the difference in reaction rates between <inline-formula><mml:math id="M315" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M316" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. The KIE values used for each oxidant are summarized in Table <xref ref-type="table" rid="T2"/>. A sensitivity analysis is conducted on the OH-KIE value, given its significant impact on the atmospheric <inline-formula><mml:math id="M317" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M318" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula><inline-formula><mml:math id="M319" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>).</p>
</sec>
<sec id="Ch1.S3.SS1.SSS5">
  <label>3.1.5</label><title>Soil sink</title>
      <p id="d2e5084">Soil uptake is a significant sink for atmospheric methane, and accounts for approximately 35 <inline-formula><mml:math id="M320" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> in the global methane budget <xref ref-type="bibr" rid="bib1.bibx111" id="paren.112"/>. Moreover, the soil sink is known to induce isotopic fractionation, which must be accounted for in forward simulations of the isotopic signal <xref ref-type="bibr" rid="bib1.bibx126" id="paren.113"/>. In this study, rather than using a fixed negative flux, we represent soil uptake as a first-order deposition process, where the deposition velocity <inline-formula><mml:math id="M321" display="inline"><mml:mrow><mml:msub><mml:mi>v</mml:mi><mml:mtext>dep</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is computed from prescribed soil fluxes and modeled surface <inline-formula><mml:math id="M322" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> concentrations. This approach allows the sink to respond to atmospheric gradients and enables a consistent application of isotopic fractionation. Representing soil uptake via a deposition velocity ensures that the isotopic fractionation is applied dynamically to both <inline-formula><mml:math id="M323" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M324" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, in proportion to their atmospheric concentrations and the kinetic isotope effect.</p>
      <p id="d2e5169">The monthly deposition velocity is calculated as:

                  <disp-formula id="Ch1.E6" content-type="numbered"><label>6</label><mml:math id="M325" display="block"><mml:mstyle displaystyle="true" class="stylechange"/><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:msub><mml:mi>v</mml:mi><mml:mtext>dep</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mtext>soil</mml:mtext></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:msub><mml:mtext>CH</mml:mtext><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:msub></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:math></disp-formula>

            where <inline-formula><mml:math id="M326" display="inline"><mml:mrow><mml:msub><mml:mi>F</mml:mi><mml:mtext>soil</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is the prior soil uptake flux from the GMB dataset <xref ref-type="bibr" rid="bib1.bibx68" id="paren.114"/>, and <inline-formula><mml:math id="M327" display="inline"><mml:mrow><mml:msub><mml:mi>C</mml:mi><mml:mrow><mml:msub><mml:mtext>CH</mml:mtext><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the modeled surface <inline-formula><mml:math id="M328" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction from inversion <xref ref-type="bibr" rid="bib1.bibx136" id="paren.115"/>.</p>
      <p id="d2e5249">To account for isotopic fractionation during methane uptake by soils, a kinetic isotope effect (KIE) is applied. The deposition velocity for <sup>13</sup><inline-formula><mml:math id="M330" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is computed as:

                  <disp-formula id="Ch1.E7" content-type="numbered"><label>7</label><mml:math id="M331" display="block"><mml:mstyle displaystyle="true" class="stylechange"/><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:msub><mml:mi>v</mml:mi><mml:mrow><mml:mtext>dep</mml:mtext><mml:mo>,</mml:mo><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mtext>CH</mml:mtext><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mi>v</mml:mi><mml:mrow><mml:mtext>dep</mml:mtext><mml:mo>,</mml:mo><mml:msup><mml:mi/><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:msub><mml:mtext>CH</mml:mtext><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mtext>KIE</mml:mtext><mml:mrow><mml:msup><mml:mi mathvariant="italic">δ</mml:mi><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:math></disp-formula>

            with a fractionation factor <inline-formula><mml:math id="M332" display="inline"><mml:mrow><mml:msub><mml:mtext>KIE</mml:mtext><mml:mrow><mml:msup><mml:mi mathvariant="italic">δ</mml:mi><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1.020</mml:mn></mml:mrow></mml:math></inline-formula>, based on the experimental results of <xref ref-type="bibr" rid="bib1.bibx126" id="text.116"/>.</p>
      <p id="d2e5354">The methodology presented in this section provides a consistent framework for simulating atmospheric <inline-formula><mml:math id="M333" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions and <inline-formula><mml:math id="M334" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M335" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M336" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signals using the CIF coupled to the LMDz transport model.</p>
</sec>
</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><title>Protocol for sensitivity experiments</title>
      <p id="d2e5406">A series of sensitivity simulations was conducted to assess the impact of key input uncertainties on the modeled spatial and temporal variability of atmospheric <inline-formula><mml:math id="M337" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M338" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M339" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal and <inline-formula><mml:math id="M340" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions. The purpose of these sensitivity experiments and the way input and output uncertainties are propagated within the inversion framework are illustrated in Fig. <xref ref-type="fig" rid="F4"/>. These experiments, summarized in Table <xref ref-type="table" rid="T3"/>, are grouped into four main categories: <list list-type="bullet"><list-item>
      <p id="d2e5456"><italic>Flux aggregation.</italic> We tested the sensitivity of modeled outputs to the choice of emission inventories used for isotopic flux aggregation. Fluxes were aggregated using different anthropogenic inventories, namely the Emissions Database for Global Atmospheric Research (EDGARv8; <xref ref-type="bibr" rid="bib1.bibx23" id="altparen.117"/>), the Global Fuel Exploitation Inventory (GFEIv2; <xref ref-type="bibr" rid="bib1.bibx112" id="altparen.118"/>), the Community Emissions Data System (CEDSv2021; <xref ref-type="bibr" rid="bib1.bibx90" id="altparen.119"/>), and the Greenhouse Gas and Air Pollution Interactions and Synergies model (GAINSv4; <xref ref-type="bibr" rid="bib1.bibx42" id="altparen.120"/>). These datasets are collectively referred to as “inventories” hereinafter. We also tested the effect of increasing the number of aggregated source categories (from 5 to 14) to assess the trade-offs between computational efficiency and isotopic detail (see Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>).</p></list-item><list-item>
      <p id="d2e5476"><italic>Chemistry.</italic> Sensitivity to <inline-formula><mml:math id="M341" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> oxidative loss processes was explored by using different OH fields, including the INCA model <xref ref-type="bibr" rid="bib1.bibx41" id="paren.121"/>, the TRANSCOM-MCFCAL ensemble <xref ref-type="bibr" rid="bib1.bibx92" id="paren.122"/>, and the IAV scenario <xref ref-type="bibr" rid="bib1.bibx93" id="paren.123"/>, as well as by varying the kinetic isotope effects (KIEs) associated with <inline-formula><mml:math id="M342" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> oxidation by OH radicals <xref ref-type="bibr" rid="bib1.bibx16 bib1.bibx108" id="paren.124"/>. Note that the other two <inline-formula><mml:math id="M343" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> oxidation pathways included in the model, Cl oxidation and soil uptake, were not independently perturbed in the sensitivity ensemble. The impact of Cl fields on modeled <inline-formula><mml:math id="M344" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M345" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M346" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M347" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> within the same LMDz-SACS framework has been comprehensively quantified by <xref ref-type="bibr" rid="bib1.bibx135" id="text.125"/>, and we adopt here the Cl field from <xref ref-type="bibr" rid="bib1.bibx145" id="text.126"/>. The soil sink, implemented as an isotope-sensitive first-order deposition process (Sect. 3.1.5), carries a well-constrained global magnitude and a moderate KIE. The implications of these two sinks for the <inline-formula><mml:math id="M348" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M349" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M350" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> budget are discussed in Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS3"/>.</p></list-item><list-item>
      <p id="d2e5606"><italic>CH</italic><sub>4</sub><italic> fluxes.</italic> Sensitivity to the choice of methane flux datasets was assessed for three sectors: wetlands (GMB climatology and interannual variability (IAV) <xref ref-type="bibr" rid="bib1.bibx68" id="paren.127"/>, LPJ from GMB <xref ref-type="bibr" rid="bib1.bibx110" id="paren.128"/>, SatWet<inline-formula><mml:math id="M352" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx9" id="paren.129"/>); freshwater systems (on/off configuration using GMB <xref ref-type="bibr" rid="bib1.bibx68" id="altparen.130"/>); and anthropogenic sources (EDGARv8, CEDSv2021, GAINSv4, GFEI).</p></list-item><list-item>
      <p id="d2e5646"><italic>Isotopic signature.</italic> For the five main source sectors, a Monte Carlo ensemble (five members) was generated to isolate the influence of source signature uncertainties on the modeled <inline-formula><mml:math id="M353" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M354" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M355" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. Isotopic signatures were randomly perturbed within their sector-specific uncertainty ranges, assumed to follow normal distributions (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS3"/>). Each spatial domain draws independently from this distribution, so that different regions may receive different perturbed values within the same Monte Carlo member. Further details, including the statistical parameters used for each sector, are provided in Table S3 in the Supplement.</p></list-item></list></p>

<table-wrap id="T3" specific-use="star"><label>Table 3</label><caption><p id="d2e5685">Overview of the simulation setups used for the sensitivity analysis. Simulations are grouped into three main categories (<italic>Category</italic>): chemistry, aggregation, and fluxes. The column <italic>Subcategory</italic> specifies the specific parameter being tested (e.g. OH fields, KIE values, wetland emissions, freshwater emissions, anthropogenic emissions). Simulation names in <italic>italic</italic> correspond to the reference simulations used in each category. Models and datasets used include: INCA <xref ref-type="bibr" rid="bib1.bibx41" id="paren.131"/>, IAV <xref ref-type="bibr" rid="bib1.bibx93" id="paren.132"/>, MCFCAL <xref ref-type="bibr" rid="bib1.bibx92" id="paren.133"/> for OH fields, Saueressig <xref ref-type="bibr" rid="bib1.bibx108" id="paren.134"/> and Cantrell <xref ref-type="bibr" rid="bib1.bibx16" id="paren.135"/> for OH kinetic isotope effects (KIE), EDGARv8 <xref ref-type="bibr" rid="bib1.bibx23" id="paren.136"/>, GFEI v2 <xref ref-type="bibr" rid="bib1.bibx112" id="paren.137"/>, CEDS v2021-04-21 <xref ref-type="bibr" rid="bib1.bibx90" id="paren.138"/>, and GAINSv4 <xref ref-type="bibr" rid="bib1.bibx42" id="paren.139"/> for anthropogenic emissions, GMB <xref ref-type="bibr" rid="bib1.bibx68" id="paren.140"/> for freshwater emissions, and various versions of wetland emissions from <xref ref-type="bibr" rid="bib1.bibx110" id="text.141"/>, including GMB_Mean (climatological mean of 11 models), GMB_NoClimato (monthly mean of 11 models), and LPJ (LPJ-wsl model). The bold font highlights, for each subcategory, the specific parameter value that is perturbed relative to the reference simulation (whose name is given in italic). </p></caption><oasis:table frame="topbot"><oasis:tgroup cols="9">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="left"/>
     <oasis:colspec colnum="5" colname="col5" align="left"/>
     <oasis:colspec colnum="6" colname="col6" align="left"/>
     <oasis:colspec colnum="7" colname="col7" align="left"/>
     <oasis:colspec colnum="8" colname="col8" align="left"/>
     <oasis:colspec colnum="9" colname="col9" align="left"/>
     <oasis:thead>
       <oasis:row>

         <oasis:entry colname="col1">Category</oasis:entry>

         <oasis:entry colname="col2">Subcategory</oasis:entry>

         <oasis:entry colname="col3">Simulation name</oasis:entry>

         <oasis:entry colname="col4">OH</oasis:entry>

         <oasis:entry colname="col5">KIE</oasis:entry>

         <oasis:entry colname="col6">Flux aggregation</oasis:entry>

         <oasis:entry rowsep="1" namest="col7" nameend="col9" align="center">Fluxes </oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col1"/>

         <oasis:entry colname="col2"/>

         <oasis:entry colname="col3"/>

         <oasis:entry colname="col4"/>

         <oasis:entry colname="col5"/>

         <oasis:entry colname="col6"/>

         <oasis:entry colname="col7">Wetlands</oasis:entry>

         <oasis:entry colname="col8">Freshwaters</oasis:entry>

         <oasis:entry colname="col9">Anthropogenic</oasis:entry>

       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>

         <oasis:entry rowsep="1" colname="col1" morerows="5">Chemistry</oasis:entry>

         <oasis:entry rowsep="1" colname="col2" morerows="3">OH</oasis:entry>

         <oasis:entry colname="col3"><italic>OH_INCA</italic></oasis:entry>

         <oasis:entry colname="col4"><bold>INCA</bold></oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">OH_IAV</oasis:entry>

         <oasis:entry colname="col4"><bold>IAV</bold></oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">OH_MCFCAL</oasis:entry>

         <oasis:entry colname="col4"><bold>MCFCAL</bold></oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col3">OH_INCA_2024</oasis:entry>

         <oasis:entry colname="col4"><bold>INCA</bold></oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry rowsep="1" colname="col2" morerows="1">KIE</oasis:entry>

         <oasis:entry colname="col3"><italic>KIE_SAUERESSIG</italic></oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5"><bold>Saueressig</bold></oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col3">KIE_CANTRELL</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5"><bold>Cantrell</bold></oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry rowsep="1" colname="col1" morerows="4">Aggregation</oasis:entry>

         <oasis:entry rowsep="1" colname="col2" morerows="4">Aggregation</oasis:entry>

         <oasis:entry colname="col3"><italic>AGGREG_EDGAR</italic></oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6"><bold>EDGAR</bold></oasis:entry>

         <oasis:entry colname="col7">GMB</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">AGGREG_GFEI</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6"><bold>GFEI</bold></oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">AGGREG_CEDS</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6"><bold>CEDS</bold></oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">AGGREG_GAINS</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6"><bold>GAINS</bold></oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col3">NO_AGGREG</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6"><bold>None</bold></oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">None</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col1" morerows="11">Fluxes</oasis:entry>

         <oasis:entry rowsep="1" colname="col2" morerows="3">Wetlands</oasis:entry>

         <oasis:entry colname="col3"><italic>WET_GMB</italic></oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7"><bold>GMB_Mean</bold></oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">WET_SAT_WET_CH4</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7"><bold>SatWetCH</bold><sub><bold>4</bold></sub></oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">WET_GMB_NO_CLIMATO</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7"><bold>GMB_NoClimato</bold></oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col3">WET_LPJ</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7"><bold>LPJ</bold></oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry rowsep="1" colname="col2" morerows="1">Freshwaters</oasis:entry>

         <oasis:entry colname="col3"><italic>FLUX_NO_FRESH</italic></oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8"><bold>No</bold></oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col3">FLUX_FRESH</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8"><bold>Yes</bold></oasis:entry>

         <oasis:entry colname="col9">EDGAR</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col2" morerows="3">Anthropogenic</oasis:entry>

         <oasis:entry colname="col3"><italic>ANTHROPO_EDGAR</italic></oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9"><bold>EDGAR</bold></oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">ANTHROPO_GAINS</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9"><bold>GAINS</bold></oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">ANTHROPO_CEDS</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9"><bold>CEDS</bold></oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col3">ANTHROPO_GFEI</oasis:entry>

         <oasis:entry colname="col4">INCA</oasis:entry>

         <oasis:entry colname="col5">Saueressig</oasis:entry>

         <oasis:entry colname="col6">EDGAR</oasis:entry>

         <oasis:entry colname="col7">GMB_Mean</oasis:entry>

         <oasis:entry colname="col8">No</oasis:entry>

         <oasis:entry colname="col9"><bold>GFEI</bold></oasis:entry>

       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d2e6403">The sensitivity analysis focuses on the period from 2016 to 2020 included. The years from 1998 to 2015 are used as a spin-up period to let the model adjust, during which the simulated atmospheric <inline-formula><mml:math id="M357" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M358" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M359" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M360" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> progressively stabilize (see Sect. S4 in the Supplement for the full 1998–2022 time series of all simulations compared to NOAA-INSTAAR observations <xref ref-type="bibr" rid="bib1.bibx75 bib1.bibx117" id="altparen.142"/>). The simulation outputs from January 2016 to December 2020 are analyzed. The years 2021–2022 are excluded to ensure consistency across all simulations, as some of the emission inventories used (e.g. GAINS) are only available up to 2020. These simulations aim to quantify the uncertainties introduced by methodological choices during the construction of isotopic signature maps and their propagation into modeled outputs, namely atmospheric methane mole fractions and isotopic signals. They also allow quantification of the individual contribution of each factor to the overall uncertainty in modeled methane mole fractions and isotopic signals.</p>
      <p id="d2e6450">The sensitivity of each parameter was quantified using the relative standard deviation (RSD), defined as:

                <disp-formula id="Ch1.E8" content-type="numbered"><label>8</label><mml:math id="M361" display="block"><mml:mstyle displaystyle="true" class="stylechange"/><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mtext>RSD</mml:mtext><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="italic">μ</mml:mi></mml:mfrac></mml:mstyle><mml:mo>×</mml:mo><mml:mn mathvariant="normal">100</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:mrow></mml:math></disp-formula>

          where <inline-formula><mml:math id="M362" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> is the standard deviation (SD) and <inline-formula><mml:math id="M363" display="inline"><mml:mi mathvariant="italic">μ</mml:mi></mml:math></inline-formula> is the mean of the modeled outputs (simulated methane mole fraction and isotopic composition) across the sensitivity simulations for a given parameter, computed at each pixel at the surface level. Both the SD and the RSD were calculated within each sensitivity category (aggregation, chemistry, fluxes, isotopic signatures) to isolate the influence of each individual parameter set on the modeled outputs.</p>
      <p id="d2e6493">The SD provides an absolute measure of dispersion (e.g. in ppb for <inline-formula><mml:math id="M364" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction values or in <inline-formula><mml:math id="M365" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>, for isotopic signals), while the RSD expresses this variability relative to the mean, allowing direct comparison between parameters of different magnitudes. An elevated RSD indicates that the modeled output is highly sensitive to the parameter in question and highlights a potential leverage point for reducing overall uncertainty. Conversely, a low RSD suggests that the parameter has only a limited impact on the variability of the output field.</p>
      <p id="d2e6515">The RSD is particularly useful in isotopic modeling, where flux amplitude, isotopic source signature, and chemical processes interact in non-linear ways. Uncertainties in the isotopic composition of a source propagate to the RSD of the modeled isotopic signal, but large fluxes from other regions with well-constrained isotopic signatures can dampen this variability.</p>
      <p id="d2e6518">The modeling framework described in this section enables a systematic exploration of the sensitivity of atmospheric <inline-formula><mml:math id="M366" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M367" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M368" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> to variations in fluxes, chemical sinks, and isotopic source signatures. We now examine the updated <inline-formula><mml:math id="M369" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M370" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M371" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps in detail and quantify their uncertainties before analyzing the results of the sensitivity simulations.</p>
</sec>
</sec>
<sec id="Ch1.S4">
  <label>4</label><title>Results and discussion</title>
      <p id="d2e6588">This section presents the key results of this study, including the spatial and temporal characteristics of the updated <inline-formula><mml:math id="M372" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M373" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M374" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps and their associated uncertainties (Sect. <xref ref-type="sec" rid="Ch1.S4.SS1"/>), as well as the atmospheric sensitivity simulations outcomes (Sect. <xref ref-type="sec" rid="Ch1.S4.SS2"/>). The objectives are to identify dominant sources of uncertainty affecting the modeled <inline-formula><mml:math id="M375" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M376" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M377" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal and to provide guidelines to integrate the updated isotopic dataset into atmospheric inversions (Sect. <xref ref-type="sec" rid="Ch1.S4.SS3"/>).</p>
<sec id="Ch1.S4.SS1">
  <label>4.1</label><title>Updated <inline-formula><mml:math id="M378" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M379" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M380" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps</title>
      <p id="d2e6693">Building updated <inline-formula><mml:math id="M381" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M382" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M383" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> maps with quantified uncertainties is a prerequisite for improving the robustness of future top-down methane budget assessments. In this section, we present the new <inline-formula><mml:math id="M384" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M385" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M386" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps developed for this study, based on the methodology detailed in Sect. <xref ref-type="sec" rid="Ch1.S2"/>. We describe the spatial patterns of aggregated sectoral signatures (Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS1"/>), their temporal variability over the 1998–2022 period (Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS2"/>), the associated uncertainties (Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS3"/>), and provide a comparison with existing datasets (Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS4"/>).</p>
<sec id="Ch1.S4.SS1.SSS1">
  <label>4.1.1</label><title>Updated <inline-formula><mml:math id="M387" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M388" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M389" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures</title>
      <p id="d2e6802">Figure <xref ref-type="fig" rid="F2"/> presents the aggregated global maps of <inline-formula><mml:math id="M390" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M391" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M392" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures averaged over the period 1998–2022. The spatial variability in these maps reflects both the diversity of isotopic signatures across sub-sectors (see Sect. <xref ref-type="sec" rid="Ch1.S1"/>) and the spatial distribution of methane fluxes within each grid cell. The fluxes used for aggregation are detailed in Table <xref ref-type="table" rid="T1"/>, which also reports the mean, minimum, and maximum <inline-formula><mml:math id="M393" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M394" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M395" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures. Additional maps showing individual sub-sectors are provided in Fig. S1 in the Supplement. The key spatial features for <inline-formula><mml:math id="M396" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M397" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M398" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> of each sector are summarized below: <list list-type="bullet"><list-item>
      <p id="d2e6901"><italic>FFG</italic>. More enriched signatures (close to <inline-formula><mml:math id="M399" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">40</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M400" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) are observed in regions with oil and gas exploitation (e.g. Middle East, USA), while more depleted values (below <inline-formula><mml:math id="M401" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M402" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) occur in coal-dominated, oil sands, or geological seepage areas (e.g. Canada). These patterns reflect the isotopic diversity of fossil sub-sources, as documented in previous studies (Figs. S1 and S2 in the Supplement; <xref ref-type="bibr" rid="bib1.bibx119 bib1.bibx122 bib1.bibx78 bib1.bibx73" id="altparen.143"/>).</p></list-item><list-item>
      <p id="d2e6946"><italic>AGW</italic>. Spatial variability results from the balance between depleted livestock emissions (<inline-formula><mml:math id="M403" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">66</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M404" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) and more enriched waste-related sources (<inline-formula><mml:math id="M405" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">51</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M406" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">56</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M407" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). Urbanized regions (e.g. South-East Asia, Europe) show enriched signatures due to dominant landfill and wastewater emissions, whereas rural areas with rice and livestock (e.g. Argentina, Sub-Saharan Africa) are more depleted (Figs. S1 and S2). Livestock signatures show notable regional variability: tropical regions tend to be more enriched (heavier than <inline-formula><mml:math id="M408" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">60</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M409" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) due to <inline-formula><mml:math id="M410" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>-dominated forage, while temperate extensive grazing systems on <inline-formula><mml:math id="M411" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> grasslands yield more depleted values. However, intensive dairy systems in the Northern Hemisphere, fed largely on <inline-formula><mml:math id="M412" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> maize silage, can also produce relatively enriched signatures <xref ref-type="bibr" rid="bib1.bibx18" id="paren.144"/>.</p></list-item><list-item>
      <p id="d2e7055"><italic>BB</italic>. Isotopic gradients are primarily latitudinal, driven by the distribution of <inline-formula><mml:math id="M413" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M414" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> plants. Tropical and subtropical regions dominated by <inline-formula><mml:math id="M415" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> vegetation exhibit more enriched values, while boreal regions show more depleted signatures <xref ref-type="bibr" rid="bib1.bibx129 bib1.bibx100 bib1.bibx55" id="paren.145"/>. Within the tropics, grass fires burning <inline-formula><mml:math id="M416" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> vegetation tend to produce more enriched <inline-formula><mml:math id="M417" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M418" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M419" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> than bush and tree fires, which involve predominantly <inline-formula><mml:math id="M420" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> biomass <xref ref-type="bibr" rid="bib1.bibx2 bib1.bibx32" id="paren.146"/>.</p></list-item><list-item>
      <p id="d2e7152"><italic>WET</italic>. Generally depleted values (<inline-formula><mml:math id="M421" display="inline"><mml:mo lspace="0mm">-</mml:mo></mml:math></inline-formula>50 to <inline-formula><mml:math id="M422" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>70 <inline-formula><mml:math id="M423" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) are observed, with more depleted signatures in high-latitude and boreal wetlands, and relatively enriched ones in tropical wetlands, where <inline-formula><mml:math id="M424" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> aquatic vegetation such as papyrus contribute to isotopically heavier signatures <xref ref-type="bibr" rid="bib1.bibx35 bib1.bibx89 bib1.bibx86 bib1.bibx32" id="paren.147"/>.</p></list-item><list-item>
      <p id="d2e7194"><italic>NAT</italic>. This sector includes geographically distinct emissions from oceans (more enriched, <inline-formula><mml:math id="M425" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">42</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M426" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) and termites (more depleted, <inline-formula><mml:math id="M427" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M428" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). The corresponding isotopic signatures reflect the spatial distribution of each sub-source, as shown in the sub-sector maps (Figs. S1 and S2).</p></list-item></list></p>

      <fig id="F2" specific-use="star"><label>Figure 2</label><caption><p id="d2e7241">Maps of <inline-formula><mml:math id="M429" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M430" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M431" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures (<inline-formula><mml:math id="M432" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) for each of the five source sectors, flux-weighted averages over 1998–2022. Only grid cells with <inline-formula><mml:math id="M433" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> fluxes exceeding 0.025 <inline-formula><mml:math id="M434" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">d</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> are shown. Note that color scales differ between panels to better highlight spatial patterns within each source sector.</p></caption>
            <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f02.png"/>

          </fig>

      <p id="d2e7330">The spatial patterns described above directly influence the simulated atmospheric <inline-formula><mml:math id="M435" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M436" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M437" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal,  which may affect the results of inverse modeling. Furthermore, uncertainties in sub-sector isotopic values and their spatial allocation propagate into regional and global inversions, ultimately influencing source attribution. A detailed quantification of these uncertainties is therefore essential to assess their potential impact and guide the design of robust inversion frameworks (Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS3"/>).</p>
      <p id="d2e7365">The maps also highlight regions where different source types co-occur, potentially complicating the separation of natural and anthropogenic emissions. For example, tropical regions such as Southeast Asia, parts of Africa, and northern South America host both WET and AGW emissions in close proximity. The spatial co-location and similarity of isotopic signatures between these sources can produce blended atmospheric signals, making it challenging to disentangle their respective contributions in top-down inversions. These overlaps underscore the importance of high-resolution spatial and temporal information in both methane fluxes and isotopic signatures to improve source attribution in complex emission environments.</p>
      <p id="d2e7368">In summary, the updated maps reveal three robust spatial features: a strong north–south gradient in BB and WET signatures driven by <inline-formula><mml:math id="M438" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>/</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:mrow></mml:math></inline-formula> vegetation distribution, a contrast between depleted livestock and enriched waste signatures within AGW, and a marked enrichment over major oil and gas basins for FFG. Regions of source overlap, particularly in the tropics, emerge as priority zones where high-resolution isotopic information is most needed for source attribution.</p>
</sec>
<sec id="Ch1.S4.SS1.SSS2">
  <label>4.1.2</label><title><inline-formula><mml:math id="M439" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M440" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M441" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature timeseries</title>
      <p id="d2e7428">Figure <xref ref-type="fig" rid="F3"/> presents the monthly <inline-formula><mml:math id="M442" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M443" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M444" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature time series for the methane sectors considered in this study over the period 1998–2022. The time series are based on flux-weighted averages. In the following, we describe the temporal evolution and variability of each sector's isotopic signature and discuss the underlying drivers. Most aggregated source sectors show limited temporal variability in their <inline-formula><mml:math id="M445" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M446" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M447" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signature over the 1998–2022 period, with typical long-term  changes below 1 <inline-formula><mml:math id="M448" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>. The isotopic signature of FFG sources exhibits a slight enrichment over time, increasing from approximately <inline-formula><mml:math id="M449" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">44.6</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M450" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> in the early 2000s to around <inline-formula><mml:math id="M451" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.9</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M452" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> after 2020. Several factors can explain this increase. First, the rapid expansion of shale gas production, particularly in North America after 2010, introduced additional emissions with relatively enriched isotopic signatures compared to conventional natural gas <xref ref-type="bibr" rid="bib1.bibx77" id="paren.148"/>. In the US, shale gas accounted for 48 <inline-formula><mml:math id="M453" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of total dry natural gas production in 2013 and reached 82 <inline-formula><mml:math id="M454" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> by 2023 <xref ref-type="bibr" rid="bib1.bibx47 bib1.bibx111" id="paren.149"/>. Second, the relative contributions of fossil fuel subsectors have evolved over the past two decades. According to <xref ref-type="bibr" rid="bib1.bibx111" id="text.150"/>, based on the synthesis of multiple emission inventories, including EDGARv6.0 and v7.0 <xref ref-type="bibr" rid="bib1.bibx29 bib1.bibx23" id="paren.151"/>, GAINSv4.0 <xref ref-type="bibr" rid="bib1.bibx42" id="paren.152"/>, CEDS <xref ref-type="bibr" rid="bib1.bibx90" id="paren.153"/>, the share of coal-related emissions, typically more depleted in <inline-formula><mml:math id="M455" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M456" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M457" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, increased from approximately 21 <inline-formula><mml:math id="M458" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of total fossil fuel emissions in the early 2000s to about 25 <inline-formula><mml:math id="M459" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> in the 2010s. Meanwhile, oil and gas emissions, associated with less depleted signatures, also grew but were partially counterbalanced by this increasing coal contribution. This sectoral shift has likely moderated the enrichment of the global signature driven by shale gas. Third, geological sources are considered stable over time, both in terms of flux and isotopic signature, providing a background that buffers the sector's temporal variability. Overall, these combined effects explain the modest but persistent enrichment observed in the FFG sector's isotopic signature over the past two decades. No significant seasonal variation is detected for FFG sector, which is consistent with the absence of seasonal modulation in the underlying inventories. However, real-world temporal variability may not be fully captured by inventories. Geopolitical events (e.g. changes in gas trade flows) and evolving gas processing or distribution practices could alter the isotopic composition of emissions over time. While isotopic signatures are generally stable <xref ref-type="bibr" rid="bib1.bibx115" id="paren.154"/>, shifts in the relative contribution of end-member sources or changes in gas composition could induce detectable trends <xref ref-type="bibr" rid="bib1.bibx118 bib1.bibx122" id="paren.155"/>. Such factors remain difficult to assess without dedicated observational constraints.</p>

      <fig id="F3" specific-use="star"><label>Figure 3</label><caption><p id="d2e7626">Monthly <inline-formula><mml:math id="M460" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M461" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M462" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures from major sectors over the period 1998–2022. Each subplot corresponds to a specific sector (AGW, WET, BB, FFG, NAT).</p></caption>
            <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f03.png"/>

          </fig>

      <p id="d2e7664">The AGW signature shows a slight enrichment from about <inline-formula><mml:math id="M463" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">60.4</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M464" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">59.9</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M465" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>. Since the isotopic values of the subcategories (e.g. livestock, wastewater, landfill, rice, and agricultural waste) are held constant, this change reflects a redistribution of fluxes within the AGW sector. Specifically, the relative contribution of livestock and rice cultivation, which together accounted for approximately 69 <inline-formula><mml:math id="M466" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of AGW emissions in 2000–2009, decreased to around 68 <inline-formula><mml:math id="M467" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> in 2010–2019. At the same time, waste-related sources (i.e. landfills, wastewater, and agricultural waste) increased from about 31 <inline-formula><mml:math id="M468" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> to 32 <inline-formula><mml:math id="M469" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of AGW emissions over the same period. This subtle but consistent shift towards more enriched waste sources likely drives the observed isotopic enrichment, particularly in rapidly developing regions with strong urban waste emissions <xref ref-type="bibr" rid="bib1.bibx111" id="paren.156"/>. Moreover, the AGW sector exhibits a seasonal cycle in its isotopic signature, primarily driven by rice cultivation, which is the only sub-sector with pronounced seasonal variability in emissions. The slight reduction in the relative contribution of rice, from about 19 <inline-formula><mml:math id="M470" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> to 16 <inline-formula><mml:math id="M471" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of total AGW emissions between 1998–2022, leads to a corresponding decrease in the seasonal amplitude of the <inline-formula><mml:math id="M472" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M473" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M474" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signature, reflecting the reduced influence of this highly seasonal sub-sector compared to other more temporally stable AGW sources. In addition to changes in source distribution, long-term shifts in agricultural practices may slightly influence isotopic source signatures. For instance, changes in livestock diet, such as a varying balance between <inline-formula><mml:math id="M475" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M476" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> feeds, and large-scale changes in atmospheric <inline-formula><mml:math id="M477" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M478" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M479" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> may both affect <inline-formula><mml:math id="M480" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> isotopic composition. <xref ref-type="bibr" rid="bib1.bibx18" id="text.157"/> showed that the progressive depletion of atmospheric <inline-formula><mml:math id="M481" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M482" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M483" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> since the 1960s, driven by fossil fuel combustion, has led to a corresponding decline in <inline-formula><mml:math id="M484" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M485" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> of both <inline-formula><mml:math id="M486" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M487" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> plants. This trend propagates through the food chain, ultimately affecting the <inline-formula><mml:math id="M488" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M489" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M490" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signature from ruminants. Although such effects likely occur, they are not yet explicitly represented in our dataset due to a lack of systematic isotopic observations that track temporal changes in agricultural feedstocks or cultivation practices.</p>
      <p id="d2e7943">The WET isotopic signature remains largely stable over the period 1998–2022, with only a minor change from approximately <inline-formula><mml:math id="M491" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">58.6</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M492" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">58.7</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M493" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>, consistent with the trend reported by <xref ref-type="bibr" rid="bib1.bibx89" id="text.158"/>. More importantly, wetlands exhibit a strong seasonal cycle in <inline-formula><mml:math id="M494" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M495" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M496" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures, with more depleted values during the summer months. This seasonal variation is driven by the dominance of methane emissions from boreal wetlands during summer, which are isotopically lighter than emissions from tropical wetlands <xref ref-type="bibr" rid="bib1.bibx89" id="paren.159"/>.</p>
      <p id="d2e8010">The BB isotopic signature remains stable around <inline-formula><mml:math id="M497" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.3</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M498" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> throughout the study period, consistent with the identical <inline-formula><mml:math id="M499" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M500" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M501" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures prescribed for biomass burning and biofuel burning subcategories <xref ref-type="bibr" rid="bib1.bibx55" id="paren.160"/>. However, the sector exhibits a pronounced seasonal cycle, with less depleted values during the boreal winter. This pattern reflects the higher contribution of biomass burning emissions from the Southern Hemisphere during this period, which are characterized by relatively enriched <inline-formula><mml:math id="M502" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M503" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M504" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures (see Fig. <xref ref-type="fig" rid="F2"/>).</p>
      <p id="d2e8095">The NAT isotopic signature remains constant throughout the period, as expected. Values for both subcategories (oceanic and termites) are derived using climatological fluxes and fixed <inline-formula><mml:math id="M505" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M506" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M507" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values, leading to negligible variability over time.</p>
      <p id="d2e8127">In summary, four sectors (FFG, AGW, BB, WET) show modest but identifiable temporal signals over 1998–2022: a slight FFG enrichment driven by shale gas expansion partially offset by rising coal contributions, a slight AGW enrichment from increasing waste shares, a stable BB mean with strong seasonal cycles, and a stable WET mean with strong boreal-summer-driven seasonality. NAT remains constant by construction. These temporal patterns are small (typically <inline-formula><mml:math id="M508" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M509" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) but systematic, and should be preserved in inversion priors.</p>
</sec>
<sec id="Ch1.S4.SS1.SSS3">
  <label>4.1.3</label><title>Uncertainty in <inline-formula><mml:math id="M510" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M511" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M512" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature</title>
      <p id="d2e8187">Table <xref ref-type="table" rid="T4"/> presents the uncertainty ranges associated with the <inline-formula><mml:math id="M513" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M514" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M515" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures for each major sector and their respective sub-sectors. The uncertainty in aggregated <inline-formula><mml:math id="M516" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M517" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M518" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures arises from two primary components: (1) the variability across sub-sectors, expressed first as the range of sub-sector uncertainties (<inline-formula><mml:math id="M519" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>), and then as a flux-weighted propagated uncertainty to the sector level (<inline-formula><mml:math id="M520" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>), and (2) the aggregation uncertainty (<inline-formula><mml:math id="M521" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>), reflecting the sensitivity of sectoral signatures to the prior flux distribution used for aggregation (see methodology in Sect. <xref ref-type="sec" rid="Ch1.S2.SS3"/>). In the following, we first analyse the uncertainty intrinsic to each sectors, then examine the additional uncertainty introduced by aggregation at the sector level, and finally discuss the total propagated uncertainties and their implications for methane source attribution.</p>

<table-wrap id="T4" specific-use="star"><label>Table 4</label><caption><p id="d2e8289">Summary of uncertainty estimates for aggregated <inline-formula><mml:math id="M522" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M523" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M524" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures by sector (in  <inline-formula><mml:math id="M525" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), based on data from 2016–2020. Sector acronyms are as follows: FFG <inline-formula><mml:math id="M526" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> Fossil Fuels and Geological sources, AGW <inline-formula><mml:math id="M527" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> Agriculture and Waste, BB <inline-formula><mml:math id="M528" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> Biomass and Biofuel Burning, WET <inline-formula><mml:math id="M529" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> Wetlands, NAT <inline-formula><mml:math id="M530" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> Other Natural sources. <inline-formula><mml:math id="M531" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> refers to the range of isotopic uncertainties across sub-sectors (in  <inline-formula><mml:math id="M532" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). These are taken from <xref ref-type="bibr" rid="bib1.bibx55" id="text.161"/> (lower bound) and <xref ref-type="bibr" rid="bib1.bibx73" id="text.162"/> (upper bound). The sub-sector uncertainty for geological sources is taken from <xref ref-type="bibr" rid="bib1.bibx27" id="text.163"/>. <inline-formula><mml:math id="M533" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> represents the sector-level propagated uncertainty, derived from the flux-weighted combination of sub-sector uncertainties. <inline-formula><mml:math id="M534" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> corresponds to the uncertainty introduced by the aggregation method, based on sensitivity tests using different prior flux inventories. <inline-formula><mml:math id="M535" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is the total combined uncertainty, calculated as <inline-formula><mml:math id="M536" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:msqrt><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:msqrt></mml:mrow></mml:math></inline-formula>. <inline-formula><mml:math id="M537" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M538" display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mtext>Uncertainty</mml:mtext><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> refer to the standard deviation and mean uncertainty reported by <xref ref-type="bibr" rid="bib1.bibx72" id="text.164"/> across all available literature. Note that since <inline-formula><mml:math id="M539" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is derived from the same base dataset, the propagated and total uncertainties (<inline-formula><mml:math id="M540" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, <inline-formula><mml:math id="M541" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) are not fully independent of <inline-formula><mml:math id="M542" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M543" display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mtext>Uncertainty</mml:mtext><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, but provide complementary comparison insight.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="8">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:colspec colnum="7" colname="col7" align="right"/>
     <oasis:colspec colnum="8" colname="col8" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">

         <oasis:entry colname="col1">Sub-sector</oasis:entry>

         <oasis:entry colname="col2"><inline-formula><mml:math id="M544" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M545" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>)</oasis:entry>

         <oasis:entry colname="col3">Sector</oasis:entry>

         <oasis:entry colname="col4"><inline-formula><mml:math id="M546" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M547" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>)</oasis:entry>

         <oasis:entry colname="col5"><inline-formula><mml:math id="M548" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M549" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>)</oasis:entry>

         <oasis:entry colname="col6"><inline-formula><mml:math id="M550" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M551" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>)</oasis:entry>

         <oasis:entry colname="col7"><inline-formula><mml:math id="M552" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M553" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>)</oasis:entry>

         <oasis:entry colname="col8"><inline-formula><mml:math id="M554" display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mtext>Uncertainty</mml:mtext><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M555" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>)</oasis:entry>

       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>

         <oasis:entry colname="col1">Coal</oasis:entry>

         <oasis:entry colname="col2">3.0–10.0</oasis:entry>

         <oasis:entry rowsep="1" colname="col3" morerows="2">FFG</oasis:entry>

         <oasis:entry rowsep="1" colname="col4" morerows="2">1.1–5.2</oasis:entry>

         <oasis:entry rowsep="1" colname="col5" morerows="2">1.0</oasis:entry>

         <oasis:entry rowsep="1" colname="col6" morerows="2">1.5–5.3</oasis:entry>

         <oasis:entry rowsep="1" colname="col7" morerows="2">9.0</oasis:entry>

         <oasis:entry rowsep="1" colname="col8" morerows="2">1.9</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col1">Oil and Gas</oasis:entry>

         <oasis:entry colname="col2">1.0–7.7</oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col1">Geological</oasis:entry>

         <oasis:entry colname="col2">1.5–1.6</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col1">Livestock</oasis:entry>

         <oasis:entry colname="col2">0.2–5.8</oasis:entry>

         <oasis:entry rowsep="1" colname="col3" morerows="4">AGW</oasis:entry>

         <oasis:entry rowsep="1" colname="col4" morerows="4">0.5–2.8</oasis:entry>

         <oasis:entry rowsep="1" colname="col5" morerows="4">1.7</oasis:entry>

         <oasis:entry rowsep="1" colname="col6" morerows="4">1.8–3.3</oasis:entry>

         <oasis:entry rowsep="1" colname="col7" morerows="4">6.5</oasis:entry>

         <oasis:entry rowsep="1" colname="col8" morerows="4">2.0</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col1">Wastewater</oasis:entry>

         <oasis:entry colname="col2">1.7–3.2</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col1">Landfills</oasis:entry>

         <oasis:entry colname="col2">1.7–3.4</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col1">Agricultural waste</oasis:entry>

         <oasis:entry colname="col2">1.7–6.6</oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col1">Rice</oasis:entry>

         <oasis:entry colname="col2">1.1–4.5</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col1">Biofuel burning</oasis:entry>

         <oasis:entry colname="col2">0.8–11.2</oasis:entry>

         <oasis:entry rowsep="1" colname="col3" morerows="1">BB</oasis:entry>

         <oasis:entry rowsep="1" colname="col4" morerows="1">0.5–6.0</oasis:entry>

         <oasis:entry rowsep="1" colname="col5" morerows="1">0.1</oasis:entry>

         <oasis:entry rowsep="1" colname="col6" morerows="1">0.5–6.0</oasis:entry>

         <oasis:entry rowsep="1" colname="col7" morerows="1">6.9</oasis:entry>

         <oasis:entry rowsep="1" colname="col8" morerows="1">1.9</oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col1">Biomass burning</oasis:entry>

         <oasis:entry colname="col2">0.8–5.2</oasis:entry>

       </oasis:row>
       <oasis:row rowsep="1">

         <oasis:entry colname="col1">Wetlands</oasis:entry>

         <oasis:entry colname="col2">0.4–8.2</oasis:entry>

         <oasis:entry colname="col3">WET</oasis:entry>

         <oasis:entry colname="col4">0.4–8.2</oasis:entry>

         <oasis:entry colname="col5">0.0</oasis:entry>

         <oasis:entry colname="col6">0.4–8.2</oasis:entry>

         <oasis:entry colname="col7">8.1</oasis:entry>

         <oasis:entry colname="col8">3.2</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col1">Oceans</oasis:entry>

         <oasis:entry colname="col2">2.8–7.6</oasis:entry>

         <oasis:entry colname="col3" morerows="1">NAT</oasis:entry>

         <oasis:entry colname="col4" morerows="1">2.0–5.4</oasis:entry>

         <oasis:entry colname="col5" morerows="1">0.0</oasis:entry>

         <oasis:entry colname="col6" morerows="1">2.0–5.4</oasis:entry>

         <oasis:entry colname="col7" morerows="1">7.6</oasis:entry>

         <oasis:entry colname="col8" morerows="1">3.2</oasis:entry>

       </oasis:row>
       <oasis:row>

         <oasis:entry colname="col1">Termites</oasis:entry>

         <oasis:entry colname="col2">2.8–7.6</oasis:entry>

       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

</sec>
<sec id="Ch1.S4.SS1.SSSx1" specific-use="unnumbered">
  <title>Propagated uncertainty from sub-sectors (<inline-formula><mml:math id="M556" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>)</title>
      <p id="d2e8945">The propagated uncertainty at the aggregated sector level, denoted <inline-formula><mml:math id="M557" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, captures the combined effect of isotopic variability among sub-sectors within each source category. It is computed using a flux-weighted combination of individual sub-sector uncertainties (<inline-formula><mml:math id="M558" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>), as described in Sect. <xref ref-type="sec" rid="Ch1.S2.SS3"/>. These sub-sector uncertainties reflect both the intrinsic heterogeneity of emission processes and the spread of values reported in the literature. The resulting <inline-formula><mml:math id="M559" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M560" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> values for each sector are summarized in Table <xref ref-type="table" rid="T4"/>. Below, we describe the dominant contributors to <inline-formula><mml:math id="M561" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, ordered from highest to lowest sectoral uncertainty.
<list list-type="bullet"><list-item>
      <p id="d2e9012">WET exhibits the largest propagated uncertainty (<inline-formula><mml:math id="M562" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.4</mml:mn></mml:mrow></mml:math></inline-formula>–<inline-formula><mml:math id="M563" display="inline"><mml:mn mathvariant="normal">8.2</mml:mn></mml:math></inline-formula> <inline-formula><mml:math id="M564" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), directly inherited from the wide range of sub-sector values (<inline-formula><mml:math id="M565" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.4</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>–8.2 <inline-formula><mml:math id="M566" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). The high variability reflects the influence of multiple environmental factors, including substrate type, methanogenic pathways (acetate fermentation vs. <inline-formula><mml:math id="M567" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> reduction), and the <inline-formula><mml:math id="M568" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M569" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> content of the organic matter <xref ref-type="bibr" rid="bib1.bibx35 bib1.bibx89" id="paren.165"/>. Tropical wetlands in particular remain under-sampled, despite representing a dominant fraction of global wetland <inline-formula><mml:math id="M570" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emissions <xref ref-type="bibr" rid="bib1.bibx31 bib1.bibx32" id="paren.166"/>.</p></list-item><list-item>
      <p id="d2e9120">BB displays a propagated uncertainty of 0.5–6.0 <inline-formula><mml:math id="M571" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>. This stems from the isotopic contrast between <inline-formula><mml:math id="M572" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M573" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> vegetation: <inline-formula><mml:math id="M574" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> plants tend to produce more enriched <inline-formula><mml:math id="M575" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M576" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M577" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> during combustion. The range of <inline-formula><mml:math id="M578" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (0.8–11.2 <inline-formula><mml:math id="M579" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) reflects differences in vegetation type across ecosystems and latitudes <xref ref-type="bibr" rid="bib1.bibx19 bib1.bibx12 bib1.bibx73" id="paren.167"/>, with tropical fire-dominated regions being particularly under-represented in isotopic measurement databases <xref ref-type="bibr" rid="bib1.bibx86" id="paren.168"/>.</p></list-item><list-item>
      <p id="d2e9220">NAT show a high sectoral uncertainty (<inline-formula><mml:math id="M580" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2.0</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>–5.4 <inline-formula><mml:math id="M581" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), driven by the strong isotopic contrast for oceanic and termite sub-sectors. Both sub-sectors exhibit broad <inline-formula><mml:math id="M582" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> values (2.8–7.6 <inline-formula><mml:math id="M583" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), reflecting limited measurement coverage and substantial environmental dependency.</p></list-item><list-item>
      <p id="d2e9270">FFG sources encompass oil, gas, coal, and geological seepage, each with distinct isotopic characteristics. The coal sub-sector, in particular, contributes significantly to the sector-level propagated uncertainty (<inline-formula><mml:math id="M584" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1.1</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>–5.2 <inline-formula><mml:math id="M585" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) due to its high variability (<inline-formula><mml:math id="M586" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">3.0</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>–10.0 <inline-formula><mml:math id="M587" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). The diversity in extraction technologies (e.g. conventional vs. unconventional gas), geological formations (e.g. shale vs. coalbed), temporal shift and regional practices leads to strong heterogeneity and uncertainty in fossil fuel signatures <xref ref-type="bibr" rid="bib1.bibx55 bib1.bibx73" id="paren.169"/>.</p></list-item><list-item>
      <p id="d2e9331">AGW exhibits the lowest sectoral propagated uncertainty among the sectors (<inline-formula><mml:math id="M588" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>–2.8 <inline-formula><mml:math id="M589" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), despite moderate to high sub-sector variability (<inline-formula><mml:math id="M590" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.2</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>–6.6 <inline-formula><mml:math id="M591" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). This is due to a flux-weighted balancing effect between well-characterized sources.</p></list-item></list></p>
      <p id="d2e9388">Beyond sectoral aggregation, the propagated uncertainties also exhibit a latitudinal structure. The distribution of <inline-formula><mml:math id="M592" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M593" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> plants drives systematic gradients in isotopic signatures across the WET, BB, and AGW sectors: tropical regions, dominated by <inline-formula><mml:math id="M594" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> vegetation, tend to produce more enriched <inline-formula><mml:math id="M595" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M596" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M597" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures, while boreal and temperate regions, where <inline-formula><mml:math id="M598" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> plants prevail, yield more depleted values <xref ref-type="bibr" rid="bib1.bibx129 bib1.bibx18 bib1.bibx32 bib1.bibx86" id="paren.170"/>. This latitudinal gradient contributes a spatially structured component to isotopic uncertainty that is not fully captured by global or regional averages.</p>
      <p id="d2e9468">These propagated uncertainties from sub-sectors highlight the need for more systematic and representative measurements, particularly in under-sampled regions (e.g. tropics), and sectors (e.g. coal mines). The scarcity of isotopic measurements in tropical regions is a critical limitation: despite hosting some of the largest <inline-formula><mml:math id="M599" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> sources globally, including tropical wetlands, rice paddies, and livestock systems, these regions remain under-represented in isotopic databases <xref ref-type="bibr" rid="bib1.bibx86 bib1.bibx32" id="paren.171"/>. Targeted field campaigns and isotopic monitoring networks could help reduce this uncertainty. Nonetheless, because of the inherent diversity and variability of methane formation processes, some degree of irreducible uncertainty must be accounted for and formally propagated in inversion frameworks (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>).</p>
</sec>
<sec id="Ch1.S4.SS1.SSSx2" specific-use="unnumbered">
  <title>Aggregation uncertainty (<inline-formula><mml:math id="M600" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>)</title>
      <p id="d2e9505">Aggregation is primarily required for computational efficiency in inversion frameworks (Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>). But, this necessary simplification introduces methodological uncertainty that must be explicitly quantified and propagated (Sect. <xref ref-type="sec" rid="Ch1.S2.SS3"/>). The aggregation uncertainty, denoted <inline-formula><mml:math id="M601" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, represents the error introduced when multiple sub-sectors are combined into a single aggregated sector based on their respective emission fluxes. The corresponding values for each sector are reported in Table <xref ref-type="table" rid="T4"/>. Although this component is generally smaller and more stable than <inline-formula><mml:math id="M602" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, it increases for sectors that involve several formation pathways and isotopic fractionation, such as FFG (1.0 <inline-formula><mml:math id="M603" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) and AGW (1.7 <inline-formula><mml:math id="M604" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), where heterogeneous sub-sector compositions lead to significant propagation effects. These values illustrate that choices made in emission inventories, not only in flux magnitudes but also in source definitions and partitioning, can significantly shape sector-level isotopic signatures.</p>
      <p id="d2e9553">Notably, discrepancies among major methane inventories, including EDGARv8 <xref ref-type="bibr" rid="bib1.bibx23" id="paren.172"/>, GAINSv4 <xref ref-type="bibr" rid="bib1.bibx42" id="paren.173"/>, CEDSv2021 <xref ref-type="bibr" rid="bib1.bibx90" id="paren.174"/>, and GFEIv2 <xref ref-type="bibr" rid="bib1.bibx112" id="paren.175"/>, contribute significantly to this aggregation uncertainty. For instance, for the FFG sector, the aggregation uncertainty is around 2.2 <inline-formula><mml:math id="M605" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> at the global scale, reflecting heterogeneity across inventories. Variability in emission factors and inventory methodologies, as described in <xref ref-type="bibr" rid="bib1.bibx111" id="text.176"/>, contribute strongly to this uncertainty. For example, oil and gas system emissions estimates vary considerably due to differences in emission factors and methodological assumptions across countries and inventories. Similarly, for the AGW sector, the aggregation uncertainty (2.8 <inline-formula><mml:math id="M606" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) reflects differences in how fluxes are allocated among agriculture and waste-related sub-sectors across inventories. For example, manure emissions can be allocated either to the agriculture or to the waste category, which can shift the aggregated isotopic signature. On the contrary, for WET, no aggregation uncertainty is reported because this sector relies on a single wetland flux dataset for weighting, precluding a cross-inventory sensitivity assessment. We note, however, that the latitudinal contrast between tropical (more enriched, <inline-formula><mml:math id="M607" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M608" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) and boreal (more depleted, <inline-formula><mml:math id="M609" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">70</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M610" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) wetlands contributes substantially to the propagated uncertainty <inline-formula><mml:math id="M611" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> already reported for this sector (0.4 <inline-formula><mml:math id="M612" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>–8.2 <inline-formula><mml:math id="M613" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). For NAT, since termite and ocean sources do not overlap geographically, the aggregation uncertainty is null.</p>
</sec>
<sec id="Ch1.S4.SS1.SSSx3" specific-use="unnumbered">
  <title>Total uncertainty (<inline-formula><mml:math id="M614" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>)</title>
      <p id="d2e9674">The total uncertainty, <inline-formula><mml:math id="M615" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, represents the combined effect of sub-sector variability and aggregation uncertainty. The full range of uncertainty values per sector (<inline-formula><mml:math id="M616" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) is reported in Table <xref ref-type="table" rid="T4"/>. This range corresponds to the spread of possible standard deviations (i.e. the uncertainty spread) rather than to a range of actual <inline-formula><mml:math id="M617" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M618" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M619" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signature values. This total uncertainty varies across sectors. For example, the BB and WET sectors exhibit wide uncertainty ranges, from 0.5 <inline-formula><mml:math id="M620" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> to 6.0 <inline-formula><mml:math id="M621" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> and from 0.4 <inline-formula><mml:math id="M622" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> to 8.2 <inline-formula><mml:math id="M623" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>, respectively, primarily driven by sub-sector uncertainties. For the BB sector, the total uncertainty is largely driven by the sub-sector variability of biofuel burning. For WET, the large uncertainty is mainly due to the inherent spatial and seasonal variability of wetland emissions. The FFG and AGW sectors show total uncertainties of up to 5.3 <inline-formula><mml:math id="M624" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> and 3.3 <inline-formula><mml:math id="M625" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>, respectively, which is consistent with their source diversity and complex sub-sector structures. NAT sources display lower average uncertainties overall.</p>
      <p id="d2e9779">The columns <inline-formula><mml:math id="M626" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> (standard deviation within the dataset) and <inline-formula><mml:math id="M627" display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mtext>Uncertainty</mml:mtext><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> (mean uncertainty) in Table <xref ref-type="table" rid="T4"/> offer a comparison with extensive literature compilations <xref ref-type="bibr" rid="bib1.bibx72" id="paren.177"/>. Our total uncertainties are comparable to or smaller than these literature-based estimates, suggesting that the applied aggregation methodology provides a structured and quantitative framework for uncertainty propagation that complements broader bibliographic syntheses. However, the sub-sector uncertainties (<inline-formula><mml:math id="M628" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) used in our calculations are derived from the same dataset compiled by <xref ref-type="bibr" rid="bib1.bibx72" id="text.178"/>. Therefore, <inline-formula><mml:math id="M629" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M630" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> are not fully independent from the comparison values in <inline-formula><mml:math id="M631" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M632" display="inline"><mml:mrow><mml:msub><mml:mover accent="true"><mml:mtext>Uncertainty</mml:mtext><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mtext>Menoud</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>. The comparison is nonetheless informative as it illustrates how the literature-based source variability propagates through our aggregation scheme.</p>
      <p id="d2e9874">These sectoral uncertainties are subsequently propagated in our sensitivity simulations (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>). They serve as a quantitative basis for defining the plausible variability ranges of source signatures, allowing us to assess their influence on modeled atmospheric <inline-formula><mml:math id="M633" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M634" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M635" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> distributions. A complementary qualitative assessment of systematic biases inherited from the underlying observational databases (e.g. uneven geographic coverage, methodological heterogeneity, limited temporal representativeness) is provided in Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS4"/>. In atmospheric inversion frameworks, the total sectoral uncertainty (<inline-formula><mml:math id="M636" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) can also be used to inform the specification of the prior error covariance matrix (<inline-formula><mml:math id="M637" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula> matrix) (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>).</p>
      <p id="d2e9931">Overall, the sectors rank by total uncertainty as WET (0.4 <inline-formula><mml:math id="M638" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>–8.2 <inline-formula><mml:math id="M639" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) <inline-formula><mml:math id="M640" display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> BB (0.5 <inline-formula><mml:math id="M641" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>–6.0 <inline-formula><mml:math id="M642" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) <inline-formula><mml:math id="M643" display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> NAT (2.0 <inline-formula><mml:math id="M644" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>–5.4 <inline-formula><mml:math id="M645" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) <inline-formula><mml:math id="M646" display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> FFG (1.5 <inline-formula><mml:math id="M647" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>–5.3 <inline-formula><mml:math id="M648" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) <inline-formula><mml:math id="M649" display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> AGW (1.8 <inline-formula><mml:math id="M650" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>–3.3 <inline-formula><mml:math id="M651" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). Sub-sector variability dominates over aggregation effects in all sectors, and the largest reducible uncertainties lie in tropical wetlands and biomass burning regions where measurements remain sparse. These sectoral uncertainties are directly used in the sensitivity simulations (Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>) and inform <inline-formula><mml:math id="M652" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula> matrix specification in inversion frameworks (Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>).</p>
</sec>
<sec id="Ch1.S4.SS1.SSS4">
  <label>4.1.4</label><title>Comparison with <inline-formula><mml:math id="M653" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M654" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M655" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> datasets from previous studies</title>
      <p id="d2e10093">For the FFG sector, our weighted mean signature is <inline-formula><mml:math id="M656" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">44.2</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>, which is generally consistent with <xref ref-type="bibr" rid="bib1.bibx55" id="text.179"/> but slightly more enriched compared to <xref ref-type="bibr" rid="bib1.bibx73" id="text.180"/> and <xref ref-type="bibr" rid="bib1.bibx136" id="text.181"/> whose values extend to more depleted ranges. Coal sources show greater differences, with our estimate around <inline-formula><mml:math id="M657" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.7</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> compared to <inline-formula><mml:math id="M658" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50.7</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> in <xref ref-type="bibr" rid="bib1.bibx73" id="text.182"/>. This discrepancy can be explained by differences in data selection criteria and spatial weighting. Our estimate is derived using flux-weighted averaging that emphasizes high-emitting coal regions, such as China and India, where emissions tend to be less depleted than the global average <xref ref-type="bibr" rid="bib1.bibx148 bib1.bibx99 bib1.bibx122 bib1.bibx55" id="paren.183"><named-content content-type="pre">e.g.</named-content></xref>. In contrast, the value reported by <xref ref-type="bibr" rid="bib1.bibx73" id="text.184"/> is an arithmetic mean of a broad compilation of site-level measurements, including more depleted coal emissions from regions with lower production or different geological contexts. The oil and gas isotopic signature is close to previous studies, with minor variation likely due to regional refinements. Geological emissions are fixed at <inline-formula><mml:math id="M659" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">46.6</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>, in line with the geochemical value from <xref ref-type="bibr" rid="bib1.bibx27" id="text.185"/>.</p>
      <p id="d2e10176">In the AGW sector, livestock methane isotopic values (<inline-formula><mml:math id="M660" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.8</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>) are more depleted than reported by <xref ref-type="bibr" rid="bib1.bibx73" id="text.186"/> (<inline-formula><mml:math id="M661" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.0</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>) and <xref ref-type="bibr" rid="bib1.bibx136" id="text.187"/> (<inline-formula><mml:math id="M662" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.6</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>). This difference likely stems from our use of the spatially explicit source signature maps from <xref ref-type="bibr" rid="bib1.bibx55" id="text.188"/>, which account for regional differences in <inline-formula><mml:math id="M663" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>/</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:mrow></mml:math></inline-formula> feed composition using global maps of biomass <inline-formula><mml:math id="M664" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow><mml:mo>/</mml:mo><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:mrow></mml:math></inline-formula> ratios <xref ref-type="bibr" rid="bib1.bibx100 bib1.bibx129" id="paren.189"/>. Flux-weighted averaging based on these maps emphasizes regions dominated by <inline-formula><mml:math id="M665" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> vegetation, such as temperate zones, resulting in more depleted signatures. Our estimate is also consistent with the <inline-formula><mml:math id="M666" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">64.9</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> value reported for 2012 by <xref ref-type="bibr" rid="bib1.bibx18" id="text.190"/>. Waste-related emissions, including landfill, wastewater, and agricultural waste, are updated following <xref ref-type="bibr" rid="bib1.bibx73" id="text.191"/>, resulting in relatively values: <inline-formula><mml:math id="M667" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50.9</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> for wastewater, <inline-formula><mml:math id="M668" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">56.2</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> for landfill, and <inline-formula><mml:math id="M669" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">54.9</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> for agricultural waste. Our landfill and wastewater values align with <xref ref-type="bibr" rid="bib1.bibx73" id="text.192"/> but differ by 2 <inline-formula><mml:math id="M670" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>–4 <inline-formula><mml:math id="M671" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> from <xref ref-type="bibr" rid="bib1.bibx55" id="text.193"/> and <xref ref-type="bibr" rid="bib1.bibx136" id="text.194"/>. This increase is attributed to changes in waste management practices, notably increased biogas production, which tends to leak methane with relatively higher <inline-formula><mml:math id="M672" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M673" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx73" id="paren.195"/>. For agricultural waste specifically, the inter-dataset spread (<inline-formula><mml:math id="M674" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">52</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M675" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">57.8</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M676" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) exceeds the sub-sector uncertainty <inline-formula><mml:math id="M677" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, pointing to genuine methodological heterogeneity in the definition of this sub-sector (crop residues vs. manure vs. composting). Rice emissions, also from <xref ref-type="bibr" rid="bib1.bibx73" id="text.196"/>, are set at <inline-formula><mml:math id="M678" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">59.9</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>, slightly more enriched than the <inline-formula><mml:math id="M679" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.0</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> used in <xref ref-type="bibr" rid="bib1.bibx136" id="text.197"/> due to differences in the amount of compiled literature.</p>
      <p id="d2e10470">For BB, our weighted mean of <inline-formula><mml:math id="M680" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.3</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> from <xref ref-type="bibr" rid="bib1.bibx55" id="text.198"/> matches closely the value from <xref ref-type="bibr" rid="bib1.bibx136" id="text.199"/>, while being slightly more depleted than in <xref ref-type="bibr" rid="bib1.bibx73" id="text.200"/>. WET signatures, derived largely from <xref ref-type="bibr" rid="bib1.bibx89" id="text.201"/>, have a weighted mean of <inline-formula><mml:math id="M681" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">58.6</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>, slightly enriched compared to <xref ref-type="bibr" rid="bib1.bibx73" id="text.202"/> (<inline-formula><mml:math id="M682" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.3</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>) and consistent with <xref ref-type="bibr" rid="bib1.bibx55" id="text.203"/>. The <inline-formula><mml:math id="M683" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">4.7</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M684" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> offset with <xref ref-type="bibr" rid="bib1.bibx73" id="text.204"/> reflects the over-representation of boreal measurements in their literature compilation vs. our flux-weighted average, which emphasizes tropical wetlands. Recent tropical airborne measurement programs report wetland source signatures of <inline-formula><mml:math id="M685" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">59.0</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>±</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mn mathvariant="normal">1.3</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M686" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> in Bolivian Amazonia <xref ref-type="bibr" rid="bib1.bibx32" id="paren.205"/> and <inline-formula><mml:math id="M687" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">59.3</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>±</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mn mathvariant="normal">2.0</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M688" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> for a Zambia–Bolivia composite <xref ref-type="bibr" rid="bib1.bibx86" id="paren.206"/>, consistent with the tropical wetland values used in our maps from <xref ref-type="bibr" rid="bib1.bibx89" id="text.207"/>. The slightly more enriched values produced by our maps over African papyrus-dominated wetlands likely reflect that these recent airborne measurements have not yet been assimilated into process-based wetland isotope models, contributing to the systematic biases on tropical wetlands discussed below.</p>
      <p id="d2e10615">Natural sources (NAT) retain previous estimates, with termites at <inline-formula><mml:math id="M689" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.4</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> and oceans at <inline-formula><mml:math id="M690" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">42.0</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>, reflecting values from <xref ref-type="bibr" rid="bib1.bibx55" id="text.208"/> and <xref ref-type="bibr" rid="bib1.bibx136" id="text.209"/>. The weighted mean of <inline-formula><mml:math id="M691" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">51.9</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> accounts for the relative contribution of these sources. For termites, we adopted a value of <inline-formula><mml:math id="M692" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.4</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>, consistent with <xref ref-type="bibr" rid="bib1.bibx55" id="text.210"/> and <xref ref-type="bibr" rid="bib1.bibx136" id="text.211"/>. The depleted signature of <inline-formula><mml:math id="M693" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">76.1</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> reported by <xref ref-type="bibr" rid="bib1.bibx131" id="text.212"/> was not used here due to concerns about potential outliers. This choice explains the discrepancy with the more depleted mean of <xref ref-type="bibr" rid="bib1.bibx73" id="text.213"/>, who included the <xref ref-type="bibr" rid="bib1.bibx131" id="text.214"/> value in their compilation.</p>
      <p id="d2e10711">Beyond these sub-sector-specific differences, the inter-dataset inconsistencies are of the same order as the sub-sector uncertainty <inline-formula><mml:math id="M694" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and point to systematic biases inherited from the underlying observational databases, which <inline-formula><mml:math id="M695" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> does not capture. At the sub-sector level, <inline-formula><mml:math id="M696" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> reflects the statistical dispersion within the sampled measurements <xref ref-type="bibr" rid="bib1.bibx73" id="paren.215"/>, not the representativeness of that sample relative to the true global distribution of emission sources. We identify three main systematic biases: <list list-type="bullet"><list-item>
      <p id="d2e10752">Uneven geographic coverage: the compilation from <xref ref-type="bibr" rid="bib1.bibx122 bib1.bibx123" id="text.216"/> underlying <xref ref-type="bibr" rid="bib1.bibx55" id="text.217"/> is dominated by North American data, EMID <xref ref-type="bibr" rid="bib1.bibx74" id="paren.218"/> improves European coverage but Africa, South America, and large parts of Asia remain under-sampled; tropical wetlands are represented through fewer campaigns than boreal/temperate ones, and recent tropical measurement programs <xref ref-type="bibr" rid="bib1.bibx32 bib1.bibx86 bib1.bibx120" id="paren.219"/> have not yet been integrated;</p></list-item><list-item>
      <p id="d2e10768">Methodological heterogeneity: literature signatures are arithmetic means while our sector values are flux-weighted;</p></list-item><list-item>
      <p id="d2e10772">Limited temporal representativeness: signatures are held constant for most sub-sectors over 1998–2022, while documented trends linked to evolving livestock feed composition or gas processing practices <xref ref-type="bibr" rid="bib1.bibx18" id="paren.220"/> are not explicitly represented.</p></list-item></list></p>
      <p id="d2e10778">The propagation of these biases to the aggregated maps depends on the flux-weighting scheme: biases affecting small-flux sub-sectors (termites, oceans) have limited impact, while those affecting high-emitting sub-sectors (livestock, oil and gas, tropical wetlands) propagate more directly to the modeled atmospheric <inline-formula><mml:math id="M697" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M698" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M699" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal, consistent with the sensitivity hierarchy reported in Table <xref ref-type="table" rid="T6"/>.</p>

<table-wrap id="T5" specific-use="star"><label>Table 5</label><caption><p id="d2e10815">Globally averaged <inline-formula><mml:math id="M700" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M701" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M702" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values (<inline-formula><mml:math id="M703" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) for each source sector, weighted by methane flux over 1998–2022. Flux-weighted mean values were calculated using a consistent methane flux dataset across sectors and years (see Table <xref ref-type="table" rid="T1"/>), but only in cases where <inline-formula><mml:math id="M704" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M705" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M706" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures vary spatially or when aggregating sub-sectors. For literature datasets (e.g. <xref ref-type="bibr" rid="bib1.bibx73" id="altparen.221"/>; spatially fixed values for <xref ref-type="bibr" rid="bib1.bibx55" id="altparen.222"/> and <xref ref-type="bibr" rid="bib1.bibx136" id="altparen.223"/>), the reported values correspond to simple arithmetic means and are not flux-weighted. Ranges in brackets indicate minimum and maximum of mean value over time. Numbers in parentheses denote the number of measurements used in the respective studies. Bold font indicates the flux-weighted “Weighted mean” rows (aggregated sector values).</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="6">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:colspec colnum="5" colname="col5" align="right"/>
     <oasis:colspec colnum="6" colname="col6" align="right"/>
     <oasis:thead>
       <oasis:row>
         <oasis:entry colname="col1">Sector</oasis:entry>
         <oasis:entry colname="col2">Sub-sector</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M709" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M710" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M711" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (This Study)</oasis:entry>
         <oasis:entry colname="col4">
                        <xref ref-type="bibr" rid="bib1.bibx73" id="text.226"/>
                      </oasis:entry>
         <oasis:entry colname="col5">
                        <xref ref-type="bibr" rid="bib1.bibx55" id="text.227"/>
                      </oasis:entry>
         <oasis:entry colname="col6">
                        <xref ref-type="bibr" rid="bib1.bibx136" id="text.228"/>
                      </oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">(<inline-formula><mml:math id="M712" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>, range)</oasis:entry>
         <oasis:entry colname="col4">(<inline-formula><mml:math id="M713" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>, N)</oasis:entry>
         <oasis:entry colname="col5">(<inline-formula><mml:math id="M714" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>, N or range)</oasis:entry>
         <oasis:entry colname="col6">(<inline-formula><mml:math id="M715" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>, range)</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">FFG</oasis:entry>
         <oasis:entry colname="col2">Coal</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M716" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.7</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M717" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">44.5</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.3</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M718" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50.7</mml:mn></mml:mrow></mml:math></inline-formula> (66)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M719" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.6</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M720" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">44.3</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.3</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M721" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">49.6</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M722" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">54.7</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">36.1</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Oil and Gas</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M723" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">44.0</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M724" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">44.1</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.8</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M725" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">44.5</mml:mn></mml:mrow></mml:math></inline-formula> (243)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M726" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.9</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M727" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">44.0</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.5</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M728" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">45.2</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M729" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">54.7</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">36.9</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Geological sources</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M730" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">46.6</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4">N/A</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M731" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:msup><mml:mn mathvariant="normal">46.6</mml:mn><mml:mo>*</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M732" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">49.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Weighted mean</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M733" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">44.2</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M734" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">44.6</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">43.9</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M735" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">45.2</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M736" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">54.7</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">36.1</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">AGW</oasis:entry>
         <oasis:entry colname="col2">Livestock</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M737" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.8</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M738" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.9</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.7</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M739" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.0</mml:mn></mml:mrow></mml:math></inline-formula> (43)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M740" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.8</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M741" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.9</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.7</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M742" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.6</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M743" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">66.8</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">60.8</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Wastewater</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M744" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50.9</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M745" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50.9</mml:mn></mml:mrow></mml:math></inline-formula> (25)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M746" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">46.7</mml:mn></mml:mrow></mml:math></inline-formula> (1)</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M747" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">48.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Landfills</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M748" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">56.2</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M749" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">56.2</mml:mn></mml:mrow></mml:math></inline-formula> (47)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M750" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">55.0</mml:mn></mml:mrow></mml:math></inline-formula> (10)</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M751" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">52.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Agricultural waste</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M752" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">54.9</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M753" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">54.9</mml:mn></mml:mrow></mml:math></inline-formula> (28)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M754" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">57.8</mml:mn></mml:mrow></mml:math></inline-formula> (5)</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M755" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">52.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Rice</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M756" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">59.9</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M757" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">59.9</mml:mn></mml:mrow></mml:math></inline-formula> (24)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M758" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">60.5</mml:mn></mml:mrow></mml:math></inline-formula> (20)</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M759" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Weighted mean</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M760" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">60.2</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M761" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">60.4</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">59.9</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M762" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">59.5</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M763" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">66.8</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">49.5</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">BB</oasis:entry>
         <oasis:entry colname="col2">Biofuel burning</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M764" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.3</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M765" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.5</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.0</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M766" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">22.7</mml:mn></mml:mrow></mml:math></inline-formula> (10)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M767" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.3</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M768" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.5</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.0</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M769" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">20.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Biomass burning</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M770" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.2</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M771" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">25.1</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">23.1</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M772" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">26.1</mml:mn></mml:mrow></mml:math></inline-formula> (30)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M773" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.2</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M774" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">25.1</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">23.1</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M775" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.3</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M776" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.9</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">20.9</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Weighted mean</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M777" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">24.3</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M778" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.7</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">23.9</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M779" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">22.7</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M780" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">24.9</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">20.9</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">WET</oasis:entry>
         <oasis:entry colname="col2">Wetlands</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M781" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">58.6</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M782" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.3</mml:mn></mml:mrow></mml:math></inline-formula> (108)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M783" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:msup><mml:mn mathvariant="normal">58.6</mml:mn><mml:mrow><mml:mo>*</mml:mo><mml:mo>*</mml:mo></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M784" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">60.9</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M785" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">74.9</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50.0</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Weighted mean</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M786" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">58.6</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M787" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">58.6</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">58.6</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M788" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">60.9</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M789" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">74.9</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50.0</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">NAT</oasis:entry>
         <oasis:entry colname="col2">Termites</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M790" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.4</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M791" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.2</mml:mn></mml:mrow></mml:math></inline-formula> (7)</oasis:entry>
         <oasis:entry colname="col5"><inline-formula><mml:math id="M792" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.4</mml:mn></mml:mrow></mml:math></inline-formula> (6)</oasis:entry>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M793" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.4</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">Oceans</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M794" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">42.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M795" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">42.0</mml:mn></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2"><bold>Weighted mean</bold></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M796" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">51.9</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M797" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">51.9</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">51.9</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
         <oasis:entry colname="col4"/>
         <oasis:entry colname="col5"/>
         <oasis:entry colname="col6"><inline-formula><mml:math id="M798" display="inline"><mml:mrow><mml:mo mathvariant="bold">-</mml:mo><mml:mn mathvariant="bold">45.5</mml:mn></mml:mrow></mml:math></inline-formula> [<inline-formula><mml:math id="M799" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">63.0</mml:mn><mml:mo>/</mml:mo><mml:mo>-</mml:mo><mml:mn mathvariant="normal">42.0</mml:mn></mml:mrow></mml:math></inline-formula>]</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><table-wrap-foot><p id="d2e10896"><sup>*</sup> Value from <xref ref-type="bibr" rid="bib1.bibx27" id="text.224"/>. <sup>**</sup> Value from <xref ref-type="bibr" rid="bib1.bibx89" id="text.225"/>.</p></table-wrap-foot></table-wrap>

<table-wrap id="T6" specific-use="star"><label>Table 6</label><caption><p id="d2e12364">Summary of the sensitivity of modeled <inline-formula><mml:math id="M800" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction and <inline-formula><mml:math id="M801" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M802" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M803" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal to key parameters at surface level over 2016–2020. Values are given as relative and absolute standard deviations (first and second number in each cell, respectively). Note that the Cl sink is not perturbed independently in this sensitivity ensemble. This impact within the same CIF–LMDz–SACS framework has been comprehensively quantified by <xref ref-type="bibr" rid="bib1.bibx135" id="text.229"/>, who report that stratospheric Cl alone contributes a <inline-formula><mml:math id="M804" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.30</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M805" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> surface enrichment in <inline-formula><mml:math id="M806" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M807" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M808" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> via stratosphere–troposphere exchange, and modifies the seasonal cycle amplitude by 10 <inline-formula><mml:math id="M809" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>–20 <inline-formula><mml:math id="M810" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> depending on latitude, see Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS3"/> for further discussion.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="3">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:colspec colnum="3" colname="col3" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Category</oasis:entry>
         <oasis:entry colname="col2">Sensitivity of <inline-formula><mml:math id="M811" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">Sensitivity of <inline-formula><mml:math id="M812" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M813" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M814" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Flux aggregation</oasis:entry>
         <oasis:entry colname="col2">0.1 <inline-formula><mml:math id="M815" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/5.6 <inline-formula><mml:math id="M816" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.3 <inline-formula><mml:math id="M817" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.06 <inline-formula><mml:math id="M818" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Fluxes</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Wetland fluxes</oasis:entry>
         <oasis:entry colname="col2">1.7 <inline-formula><mml:math id="M819" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/25.2 <inline-formula><mml:math id="M820" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.9 <inline-formula><mml:math id="M821" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.18 <inline-formula><mml:math id="M822" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Freshwater fluxes</oasis:entry>
         <oasis:entry colname="col2">1.4 <inline-formula><mml:math id="M823" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/67.8 <inline-formula><mml:math id="M824" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.9 <inline-formula><mml:math id="M825" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.21 <inline-formula><mml:math id="M826" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Anthropogenic fluxes</oasis:entry>
         <oasis:entry colname="col2">2.4 <inline-formula><mml:math id="M827" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/30.1 <inline-formula><mml:math id="M828" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.6 <inline-formula><mml:math id="M829" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.29 <inline-formula><mml:math id="M830" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Chemistry</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">OH fields</oasis:entry>
         <oasis:entry colname="col2">3.6 <inline-formula><mml:math id="M831" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/49.6 <inline-formula><mml:math id="M832" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.0 <inline-formula><mml:math id="M833" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.02 <inline-formula><mml:math id="M834" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">OH Kinetic Isotope Effect (KIE)</oasis:entry>
         <oasis:entry colname="col2">0.0 <inline-formula><mml:math id="M835" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.0 <inline-formula><mml:math id="M836" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">2.2 <inline-formula><mml:math id="M837" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.40 <inline-formula><mml:math id="M838" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Source signature</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3"/>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Fossil Fuel and Geological (FFG)</oasis:entry>
         <oasis:entry colname="col2">0.0 <inline-formula><mml:math id="M839" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.0 <inline-formula><mml:math id="M840" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.4 <inline-formula><mml:math id="M841" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.04 <inline-formula><mml:math id="M842" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Agriculture and Waste (AGW)</oasis:entry>
         <oasis:entry colname="col2">0.0 <inline-formula><mml:math id="M843" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.0 <inline-formula><mml:math id="M844" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">1.7 <inline-formula><mml:math id="M845" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.32 <inline-formula><mml:math id="M846" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Biomass Burning (BB)</oasis:entry>
         <oasis:entry colname="col2">0.0 <inline-formula><mml:math id="M847" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.0 <inline-formula><mml:math id="M848" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.8 <inline-formula><mml:math id="M849" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.16 <inline-formula><mml:math id="M850" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Natural Sources (NAT)</oasis:entry>
         <oasis:entry colname="col2">0.0 <inline-formula><mml:math id="M851" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.0 <inline-formula><mml:math id="M852" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.4 <inline-formula><mml:math id="M853" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.07 <inline-formula><mml:math id="M854" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Wetlands (WET)</oasis:entry>
         <oasis:entry colname="col2">0.0 <inline-formula><mml:math id="M855" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.0 <inline-formula><mml:math id="M856" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">0.1 <inline-formula><mml:math id="M857" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>/0.02 <inline-formula><mml:math id="M858" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

      <p id="d2e13039">Generally, the updated <inline-formula><mml:math id="M859" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M860" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M861" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps show clear sectoral and regional patterns, with depleted signatures for wetlands and agriculture, and enriched signatures for fossil fuel and biomass burning emissions. Temporal variations are limited over the study period, except in sectors where emissions were known to vary in time. Uncertainty analysis highlights significant variability, particularly for the agriculture and waste sector. The updated maps are broadly consistent with recent datasets. In the next section, we assess how the uncertainties over inputs propagate to the modeled atmospheric <inline-formula><mml:math id="M862" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M863" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M864" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal through sensitivity simulations.</p>
</sec>
</sec>
<sec id="Ch1.S4.SS2">
  <label>4.2</label><title>Sensitivity of simulated atmospheric <inline-formula><mml:math id="M865" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M866" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M867" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal and <inline-formula><mml:math id="M868" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions to key parameters</title>
      <p id="d2e13150">Forward atmospheric simulations provide a framework for assessing the impact of source signature uncertainties on modeled <inline-formula><mml:math id="M869" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M870" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M871" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS1"/>). By testing several sets of key input parameters (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>), we can identify which sources of uncertainty have the strongest influence on the atmospheric isotopic signal. This approach, and the way input and output uncertainties are propagated within the inversion framework, is illustrated in Fig. <xref ref-type="fig" rid="F4"/>. In this section, we evaluate the sensitivity of simulated atmospheric <inline-formula><mml:math id="M872" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions and <inline-formula><mml:math id="M873" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M874" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M875" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> isotopic signals  at the surface, where observations are available, to key parameters, including emission inventories for aggregation (Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS1"/>), fluxes (Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS2"/>), chemical reactions (Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS3"/>), and source signatures (Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS4"/>). Table <xref ref-type="table" rid="T6"/> provides a comparative overview of the sensitivities, allowing a quick identification of which parameters most influence the modeled <inline-formula><mml:math id="M876" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions and isotopic signals. Detailed results and interpretations are provided in the following sub-sections.</p>

      <fig id="F4" specific-use="star"><label>Figure 4</label><caption><p id="d2e13253">In the upper panel, coloured Gaussian curves (yellow: prior, blue: observation, green: posterior) illustrate how the ratio between  <inline-formula><mml:math id="M877" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula> (prior error covariance matrix) and  <inline-formula><mml:math id="M878" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> (observation error covariance matrix) determines the strength of the inversion constraint: (i) when  <inline-formula><mml:math id="M879" display="inline"><mml:mrow><mml:mi mathvariant="bold">B</mml:mi><mml:mo>≈</mml:mo><mml:mi mathvariant="bold">R</mml:mi></mml:mrow></mml:math></inline-formula>, the optimal balance yields the strongest constraint; (ii) when  <inline-formula><mml:math id="M880" display="inline"><mml:mrow><mml:mi mathvariant="bold">B</mml:mi><mml:mo>≫</mml:mo><mml:mi mathvariant="bold">R</mml:mi></mml:mrow></mml:math></inline-formula>, observations dominate and the posterior approaches the observations; (iii) when  <inline-formula><mml:math id="M881" display="inline"><mml:mrow><mml:mi mathvariant="bold">B</mml:mi><mml:mo>≪</mml:mo><mml:mi mathvariant="bold">R</mml:mi></mml:mrow></mml:math></inline-formula>, the prior dominates and the posterior remains close to the prior. The middle panel conceptually shows how uncertainties are quantified in the sensitivity framework. Input uncertainties determine which constraint case applies and how to set  <inline-formula><mml:math id="M882" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula> in the parameter space, which is mapped into the concentration space by the atmospheric model operator <inline-formula><mml:math id="M883" display="inline"><mml:mrow><mml:mi mathvariant="script">H</mml:mi><mml:mo>(</mml:mo><mml:mi>x</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>. Output uncertainties indicate the reliability of the inversion results; if too high, results are not robust. They can be reduced through improved priors or explicitly optimized within the inversion framework. The bottom panel summarises how these uncertainties are formalised within the  <inline-formula><mml:math id="M884" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula> matrix and the  <inline-formula><mml:math id="M885" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> matrix.</p></caption>
          <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f04.png"/>

        </fig>

<sec id="Ch1.S4.SS2.SSS1">
  <label>4.2.1</label><title>Sensitivity to fluxes used for aggregation</title>
      <p id="d2e13355">We note that the term “aggregation” is used in two distinct methodological senses in this section. The first refers to the choice of flux inventory used to weight sub-sector isotopic signatures into sector-level values, which generates the aggregation uncertainty <inline-formula><mml:math id="M886" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> reported in Table <xref ref-type="table" rid="T4"/> (AGGREG_EDGAR, AGGREG_GFEI, AGGREG_CEDS and AGGREG_GAINS simulations). The second refers to the sectoral granularity of the atmospheric model itself, i.e. the number of source categories effectively transported (5 by default vs. 14 in the NO_AGGREG simulation). Both are tested below but answer complementary questions: the former probes the sensitivity of the aggregated signature values, while the latter probes the sensitivity of the modeled atmospheric signal to the level of sub-sector resolution.</p>
      <p id="d2e13371">Figure <xref ref-type="fig" rid="F5"/> summarizes the sensitivity of flux aggregation to different prior datasets. Panel (a) shows the variability of flux estimates between inventories, highlighting where emission fluxes are most uncertain. Since this test focuses specifically on uncertainties arising from the flux-weighted aggregation of isotopic signatures, only anthropogenic sectors (FFG, AGW and BB) are included (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>). Panel (b) presents the resulting variability in the aggregated <inline-formula><mml:math id="M887" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M888" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M889" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures by sector. Panel (c) shows the sensitivity of simulated atmospheric <inline-formula><mml:math id="M890" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M891" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M892" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signals to these aggregated isotopic changes at surface level. It is important to note that panel (c) displays a single sensitivity map representing the combined impact of flux-weighted isotopic signatures variations across all anthropogenic sectors on isotopic signal simulated at the surface. Because only isotopic signatures are perturbed while the underlying emission fluxes remain unchanged, this test does not directly affect <inline-formula><mml:math id="M893" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions. The only noticeable effect on <inline-formula><mml:math id="M894" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions occurs in the “NO_AGGREG” setup, in which the number of aggregated source categories was increased from 5 to 14 to evaluate the impact of the trade-offs between computational efficiency and isotopic detail (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>), resulting in a very small change in simulated <inline-formula><mml:math id="M895" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions (about 5.6 <inline-formula><mml:math id="M896" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> on average; Table <xref ref-type="table" rid="T6"/>). Figure S3 in the Supplement shows the same information as in Fig. <xref ref-type="fig" rid="F5"/> but expressed in terms of relative standard deviation (RSD). Together, these results illustrate how inventory discrepancies propagate through to atmospheric simulations of <inline-formula><mml:math id="M897" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M898" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M899" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal.</p>

      <fig id="F5" specific-use="star"><label>Figure 5</label><caption><p id="d2e13516"><bold>(a)</bold> SD (in <inline-formula><mml:math id="M900" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) of the fluxes among different prior datasets (GAINSv4, CEDSv2021, GFEIv2, EDGARv8) (over 2016–2020) at surface level. Values are only displayed when the associated <inline-formula><mml:math id="M901" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> flux is higher than 0.2 <inline-formula><mml:math id="M902" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">d</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, for aggregated categories. <bold>(b)</bold> SD in <inline-formula><mml:math id="M903" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> of the <inline-formula><mml:math id="M904" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M905" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M906" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature by aggregated category at surface level. <bold>(c)</bold> SD in <inline-formula><mml:math id="M907" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> of the <inline-formula><mml:math id="M908" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M909" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M910" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signals from the forward model outputs at surface level. Coloured circles indicate SD of observed <inline-formula><mml:math id="M911" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M912" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M913" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values at each surface station over the study period <xref ref-type="bibr" rid="bib1.bibx75 bib1.bibx117" id="paren.230"/>.</p></caption>
            <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f05.png"/>

          </fig>

      <p id="d2e13711">The largest flux uncertainties (Fig. S3a in the Supplement) are observed in the Fossil Fuels and Geological (FFG) and Agriculture and Waste (AGW) sectors (65 <inline-formula><mml:math id="M914" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> and 41 <inline-formula><mml:math id="M915" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> respectively). These uncertainties stem from differences between inventories, which exhibit regional discrepancies. For example, in Central Asia (Turkmenistan, Afghanistan, Uzbekistan), there are significant differences in fossil fuel emission estimates. In Turkmenistan, GAINS estimates 1259 <inline-formula><mml:math id="M916" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kt</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, while EDGARv8 and CEDS report 1343 and 1351 <inline-formula><mml:math id="M917" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kt</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> respectively and GFEI 888 <inline-formula><mml:math id="M918" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kt</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. Although totals appear similar, the spatial allocation and sectoral breakdown differ markedly between inventories. This is partly because inventories rely on national reports submitted to the UNFCCC, ensuring consistency at the country level but not necessarily in spatial detail or sub-sector attribution. Additionally, satellite-based studies (e.g. <xref ref-type="bibr" rid="bib1.bibx144" id="altparen.231"/>) have identified emission events in regions such as Turkmenistan, associated with fossil fuel infrastructure. However, such episodic or localized emissions are generally not included in bottom-up inventories, which may underestimate the true emission rates. In the AGW sector, a high RSD is observed in Botswana. This is linked to the aggregation structure in GAINS,  where large African regions are aggregated, whereas other inventories provide country-level estimates.</p>
      <p id="d2e13804">The impact of these flux uncertainties on <inline-formula><mml:math id="M919" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M920" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M921" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures (Fig. <xref ref-type="fig" rid="F5"/>b) is especially pronounced in the AGW sector, which shows the highest isotopic sensitivity (1.7 <inline-formula><mml:math id="M922" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), particularly in the Middle East and parts of Africa. This is related to the relative contributions of sub-sectors with distinct isotopic signatures, such as livestock (more depleted) and waste (less depleted), as defined in the inventories. For instance, in Ethiopia (2016–2020), livestock accounts for 79 <inline-formula><mml:math id="M923" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of AGW emissions in CEDS and GAINS, but only 67 <inline-formula><mml:math id="M924" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> in EDGARv8, which is reflected in the region's isotopic signature variability. Regional variations in livestock diets, driven by the local balance between <inline-formula><mml:math id="M925" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M926" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> forage plants, further contribute to this spread <xref ref-type="bibr" rid="bib1.bibx18" id="paren.232"/>. For instance, in Ethiopia, the balance between <inline-formula><mml:math id="M927" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M928" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> forage grasses varies with altitude, leading to distinct isotopic signatures within the same country <xref ref-type="bibr" rid="bib1.bibx13" id="paren.233"/>. AGW is disaggregated in our framework into five sub-sectors (livestock, rice, landfills, wastewater, and agricultural waste; Table <xref ref-type="table" rid="T1"/>), each with its own isotopic signature and flux distribution. Livestock and rice together account for <inline-formula><mml:math id="M929" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">62</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M930" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of AGW emissions and carry the most depleted signatures (<inline-formula><mml:math id="M931" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.8</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M932" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M933" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">59.9</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M934" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), while waste-related sub-sectors (<inline-formula><mml:math id="M935" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50.9</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M936" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">56.2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M937" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) make up the remaining 38 <inline-formula><mml:math id="M938" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>. This contrast is the main driver of the propagated uncertainty <inline-formula><mml:math id="M939" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>prop</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> reported for AGW in Table <xref ref-type="table" rid="T4"/>. To assess whether finer sectoral granularity, i.e. the number of source categories effectively resolved in the atmospheric model, would meaningfully change the modeled atmospheric signal, the NO_AGGREG simulation increases the number of source categories from 5 to 14 (Table <xref ref-type="table" rid="T3"/>). This is conceptually distinct from the aggregation uncertainty <inline-formula><mml:math id="M940" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> defined in Sect. <xref ref-type="sec" rid="Ch1.S2.SS3.SSS3"/>, which quantifies the sensitivity of the aggregated signature to the choice of flux inventory used for weighting (Fig. <xref ref-type="fig" rid="F5"/>). The resulting differences are small: <inline-formula><mml:math id="M941" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.061</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M942" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> globally for <inline-formula><mml:math id="M943" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M944" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M945" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (Fig. S4 in the Supplement). Localized differences of up to <inline-formula><mml:math id="M946" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M947" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> in <inline-formula><mml:math id="M948" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M949" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M950" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> occur in regions where sub-sector composition contrasts strongly with the global average, notably in South Asia and the Middle East. These results indicate that increasing sectoral granularity beyond five sub-sectors does not substantially alter the modeled atmospheric isotopic signal at the global scale. Reducing AGW-related uncertainty would therefore benefit more from better-constraining  the signature values of the existing sub-sectors and from refining inventory-level flux partitioning between livestock and waste, particularly in rapidly developing regions, than from increasing the number of source categories.</p>
      <p id="d2e14134">In contrast, the FFG sector shows lower isotopic sensitivity despite higher flux uncertainties (2.2 <inline-formula><mml:math id="M951" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>). This is explained by the more homogeneous isotopic signatures of coal, oil and gas and geological, and the smaller relative isotopic differences among sub-sectors. The uncertainties are highest in North America, they are mainly associated with the difference in relative contribution of oil and gas vs. coal in the datasets. The variability in Chinese coal emissions is also well documented, with CEDS based on EDGARv4.2 previously overestimating emissions compared to recent regional inventories <xref ref-type="bibr" rid="bib1.bibx63 bib1.bibx111" id="paren.234"/>. These results highlight the key role of emission partitioning within aggregated categories in shaping the final isotopic source signature, particularly in the AGW sector. These uncertainty values are used to define the <inline-formula><mml:math id="M952" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> parameter in the uncertainty analysis (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS1.SSS3"/>).</p>
      <p id="d2e14161">The sensitivity of simulated atmospheric <inline-formula><mml:math id="M953" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M954" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M955" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signals to aggregation choices remains globally low, with a mean RSD of 0.32 <inline-formula><mml:math id="M956" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> (Fig. S3c in the Supplement) and a mean SD of approximately 0.06 <inline-formula><mml:math id="M957" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (Fig. <xref ref-type="fig" rid="F5"/>c). This suggests that, despite regional discrepancies, aggregation uncertainties have a limited impact on large-scale atmospheric isotopic patterns. Moreover, the values shown in Fig. S3c represent relative sensitivities computed over the entire model domain, which tends to dilute localized sensitivity hotspots. When compared to the RSD of observed <inline-formula><mml:math id="M958" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M959" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M960" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values at surface stations <xref ref-type="bibr" rid="bib1.bibx75 bib1.bibx117" id="paren.235"><named-content content-type="pre">e.g.</named-content></xref>, the simulated sensitivities is smaller. This indicates that real-world atmospheric variability exceeds the response induced by inventory-driven aggregation uncertainties, and further support the limited impact of this specific error source on the modelisation of the atmospheric isotopic signal at observational sites (more details in Sect. <xref ref-type="sec" rid="Ch1.S4.SS3"/>).</p>
      <p id="d2e14248">In summary, two distinct aggregation-related effects have been tested in this section. First, the choice of flux inventory used to weight sub-sector signatures (the aggregation uncertainty <inline-formula><mml:math id="M961" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>agg</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>) introduces sizeable variability in the aggregated signature values themselves, notably for AGW and FFG, but propagates only weakly to the modeled atmospheric <inline-formula><mml:math id="M962" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M963" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M964" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal. Second, increasing the sectoral granularity from 5 to 14 source categories (NO_AGGREG test) modifies the modeled signal by only <inline-formula><mml:math id="M965" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.06</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M966" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> globally. Both aggregation-related choices therefore have a limited impact on atmospheric simulations, supporting the transferability of the updated maps across inversion systems and inventories.</p>
</sec>
<sec id="Ch1.S4.SS2.SSS2">
  <label>4.2.2</label><title>Sensitivity to uncertainties in methane fluxes from wetlands, freshwaters, and anthropogenic sectors</title>
      <p id="d2e14318">Figure <xref ref-type="fig" rid="F6"/> summarizes the sensitivity of atmospheric simulations to uncertainties in methane flux estimates from key source sectors: wetlands, freshwaters, and the total anthropogenic emissions (i.e. the sum of all anthropogenic sources). Unlike the previous section, where only isotopic signatures were perturbed through flux-weighted aggregation, here the underlying emission fluxes themselves are varied in the model simulations. Panel (a) shows the SD of <inline-formula><mml:math id="M967" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emissions across inventories, and highlight where flux uncertainties are the greatest. For a detailed breakdown of anthropogenic subsectors (e.g. fossil fuels, waste, agriculture), refer to Figs. S6 and S7 in the Supplement, which show their individual contributions. Panels (c) and (e) display the impact of uncertainties in wetlands, freshwaters, and anthropogenic fluxes on modeled <inline-formula><mml:math id="M968" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions and <inline-formula><mml:math id="M969" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M970" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M971" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signals, respectively, at surface level. Figure S5 in the Supplement shows the same information in terms of RSD. Theses figures show how uncertainties in sectoral emissions propagate into atmospheric simulations.</p>

      <fig id="F6" specific-use="star"><label>Figure 6</label><caption><p id="d2e14376">Standard deviation (SD) over 2016–2020. <bold>(a)</bold> SD (in <inline-formula><mml:math id="M972" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">kg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">s</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) of <inline-formula><mml:math id="M973" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emissions from wetlands, freshwaters, and anthropogenic sectors (AGW, FFG, BB) at surface level. Values are only displayed when the associated <inline-formula><mml:math id="M974" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> flux exceeds 0.2 <inline-formula><mml:math id="M975" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">mg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">d</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>. <bold>(b)</bold> SD (in <inline-formula><mml:math id="M976" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">molec</mml:mi><mml:mo>.</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) of the total tropospheric OH column (pressure levels below 250 <inline-formula><mml:math id="M977" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>). <bold>(c)</bold> SD (in ppb) of <inline-formula><mml:math id="M978" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions at surface level from forward model outputs, driven by uncertainty in emission fluxes. Coloured circles indicate RSD of observed <inline-formula><mml:math id="M979" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions at surface stations with co-located <inline-formula><mml:math id="M980" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M981" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>(<inline-formula><mml:math id="M982" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) measurements. <bold>(d)</bold> Same as <bold>(c)</bold>, but driven by uncertainty in OH fields. <bold>(e)</bold> SD (in <inline-formula><mml:math id="M983" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) of <inline-formula><mml:math id="M984" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M985" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M986" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values at surface level from forward model outputs, driven by uncertainty in emission fluxes. Coloured circles indicate RSD of observed <inline-formula><mml:math id="M987" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M988" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M989" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values at the same stations <xref ref-type="bibr" rid="bib1.bibx75 bib1.bibx117" id="paren.236"/>. <bold>(f)</bold> Same as <bold>(e)</bold>, but driven by uncertainty in kinetic isotope effects (KIE) during <inline-formula><mml:math id="M990" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> oxidation.</p></caption>
            <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f06.png"/>

          </fig>

      <p id="d2e14651">Methane flux uncertainties are highest for anthropogenic sources (mean RSD of 129 <inline-formula><mml:math id="M991" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), followed by wetlands (96 <inline-formula><mml:math id="M992" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) and freshwaters (22 <inline-formula><mml:math id="M993" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) (Fig. S5a in the Supplement). These differences arise from inventory discrepancies, the inherent complexity of methane emission processes (e.g. large spatio-temporal variability, dependence on environmental conditions and management practices), and the uneven availability of observational data across regions and sectors, which limits the capacity to constrain emissions. Among anthropogenic subsectors, fossil fuels exhibit the largest uncertainty (RSD 83.8 <inline-formula><mml:math id="M994" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>, Fig. S6), driven by inconsistent national reporting, the use of variable emission factors, and the presence of poorly constrained super-emitters <xref ref-type="bibr" rid="bib1.bibx60 bib1.bibx111" id="paren.237"/>. Waste emissions follow (RSD 51.9 <inline-formula><mml:math id="M995" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), and include landfills, agricultural waste, and wastewater. The limited spread across inventories for landfills is mostly due to the use of similar Tier 1 methods and data sources, not better emission constraints. Substantial uncertainties persist due to variations in emissions arising from different climate conditions, landfill management practices, and the inherent temporal and geographical variability of landfill emissions <xref ref-type="bibr" rid="bib1.bibx54 bib1.bibx84 bib1.bibx85 bib1.bibx11 bib1.bibx146" id="paren.238"/>. Wastewater emissions remain particularly uncertain due to variability in treatment processes and limited measurements <xref ref-type="bibr" rid="bib1.bibx111" id="paren.239"/>. Biofuel burning shows a high RSD (55.7 <inline-formula><mml:math id="M996" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) but low absolute impact due to its smaller flux. Agriculture (RSD 42.2 <inline-formula><mml:math id="M997" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) contributes significantly in absolute terms due to its large emissions. Regarding natural sources, wetland emission uncertainties stem from multiple factors: inconsistent wetland extent maps <xref ref-type="bibr" rid="bib1.bibx71 bib1.bibx10" id="paren.240"/>, uncertainties in methane production and oxidation modeling <xref ref-type="bibr" rid="bib1.bibx53" id="paren.241"/>, and the influence of environmental drivers such as temperature and water table depth <xref ref-type="bibr" rid="bib1.bibx138 bib1.bibx97" id="paren.242"/>. The dominant source of long-term uncertainty is wetland areal extent <xref ref-type="bibr" rid="bib1.bibx97 bib1.bibx51" id="paren.243"/>, while seasonal variability is primarily driven by meteorology <xref ref-type="bibr" rid="bib1.bibx91 bib1.bibx69" id="paren.244"/>. Tropical wetlands remain particularly uncertain due to sparse data coverage despite their importance for global feedbacks <xref ref-type="bibr" rid="bib1.bibx81 bib1.bibx151 bib1.bibx32" id="paren.245"/>. Freshwater emissions are also uncertain due to poorly mapped inland waters, complex seasonal dynamics, and diverse emission pathways (e.g. diffusion, ebullition, plant-mediated transport) <xref ref-type="bibr" rid="bib1.bibx141 bib1.bibx59 bib1.bibx111" id="paren.246"/>. However, as only one freshwater dataset was available the sensitivity shown here reflects the introduction of freshwater emissions into the simulation (ON/OFF comparison) rather than a quantified uncertainty across multiple estimates.</p>
      <p id="d2e14743">Panel (c) of Fig. <xref ref-type="fig" rid="F6"/> shows how flux uncertainties propagate into modeled <inline-formula><mml:math id="M998" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions. The strongest sensitivity is linked to freshwater emissions, with an average variability of 68 <inline-formula><mml:math id="M999" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> (4.4 <inline-formula><mml:math id="M1000" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>). This reflects a significant contribution to total methane emissions (<inline-formula><mml:math id="M1001" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">53</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1002" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>) and strong regional impacts, particularly near the Caspian Sea, where freshwater sources dominate and where no wetland or oceanic fluxes were present in the reference simulation, thus amplifying the local sensitivity (Fig. S2). The Caspian Sea is a large endorheic saline lake whose emissions are treated as freshwater in our framework given the absence of a dedicated dataset; its brackish nature and proximity to major oil and gas infrastructure introduce additional uncertainty in this region. Anthropogenic fluxes contribute to a variability of 30 <inline-formula><mml:math id="M1003" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> (2.4 <inline-formula><mml:math id="M1004" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), especially in major fossil fuel production regions such as Siberia and industrialized areas like Eastern China. Wetland fluxes result in a variability of 25 <inline-formula><mml:math id="M1005" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> (1.7 <inline-formula><mml:math id="M1006" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), concentrated in high-emission regions such as the Amazon, Southeast Asia, and the Congo Basin.</p>
      <p id="d2e14841">Similarly, modeled <inline-formula><mml:math id="M1007" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1008" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1009" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signals (panel e) show a spatial pattern that mirrors <inline-formula><mml:math id="M1010" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction sensitivity. Wetland and freshwater flux uncertainties both lead to an average isotopic variability of 0.2 <inline-formula><mml:math id="M1011" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (0.9 <inline-formula><mml:math id="M1012" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), while anthropogenic fluxes cause 0.3 <inline-formula><mml:math id="M1013" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (1.6 <inline-formula><mml:math id="M1014" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>). These findings emphasize that sectoral flux uncertainties substantially influence regional isotopic signal, particularly in areas with high methane emissions.</p>
      <p id="d2e14917">Observed SDs from surface monitoring sites (shown as colored circles) are also displayed in panels (c) and (e) for comparison. In several cases, modeled isotopic sensitivities exceed the observed SD, especially for freshwater, induced <inline-formula><mml:math id="M1015" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> variability, highlighting their relevance for inversion performance (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>). As illustrated in panels (c) and (e), the maps convey two layers of information: regional hotspots where large uncertainties may hamper local flux attribution (e.g. Caspian region, Chinese industrial basins, Congo wetlands, etc.), and background sensitivity over well-mixed or remote areas, which are critical for constraining hemispheric to global budgets. This distinction is further discussed in Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>.</p>
      <p id="d2e14935">In summary, freshwater fluxes dominate the <inline-formula><mml:math id="M1016" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction sensitivity, followed by anthropogenic and wetland fluxes. For <inline-formula><mml:math id="M1017" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1018" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1019" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, anthropogenic fluxes induce the largest variability, with wetland and freshwater contributions of similar order. Sectoral flux uncertainties produce both regional hotspots (Caspian, Congo, Chinese basins) and broader background sensitivities, both relevant for inversion design.</p>
</sec>
<sec id="Ch1.S4.SS2.SSS3">
  <label>4.2.3</label><title>Sensitivity to atmospheric chemistry parameters</title>
      <p id="d2e14986">Figure <xref ref-type="fig" rid="F6"/> also illustrates the uncertainties related to atmospheric chemistry parameters, focusing mainly on the kinetic isotope effect (KIE) of methane oxidation by tropospheric hydroxyl radicals (OH), which are the primary oxidant of methane. Panel (b) presents the SD of the total tropospheric OH column (pressure levels below 250 <inline-formula><mml:math id="M1020" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">hPa</mml:mi></mml:mrow></mml:math></inline-formula>), highlighting regions with the largest OH uncertainties. Panel (d) shows how these uncertainties affect modeled <inline-formula><mml:math id="M1021" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions at surface level. Panel (f) displays how uncertainty over KIE impacts atmospheric <inline-formula><mml:math id="M1022" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1023" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1024" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signals. OH uncertainty does not affect <inline-formula><mml:math id="M1025" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1026" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1027" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal, and OH-KIE does not impact <inline-formula><mml:math id="M1028" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions. Figure S4 shows the same information in terms of RSD.</p>
      <p id="d2e15080">Uncertainties in OH fields (Fig. <xref ref-type="fig" rid="F6"/>b and Fig. S5b in the Supplement) are substantial <xref ref-type="bibr" rid="bib1.bibx80 bib1.bibx22 bib1.bibx152 bib1.bibx128" id="paren.247"><named-content content-type="pre">e.g.</named-content></xref>. SD are particularly high over tropical continental regions such as Amazonia, South Asia, and the African savannas, where OH concentrations peak due to intense photochemistry and high humidity and where strong inter-model differences coexist <xref ref-type="bibr" rid="bib1.bibx152" id="paren.248"/>. These regions also display marked longitudinal contrasts in tropospheric OH, driven by zonal asymmetries in convection, lightning <inline-formula><mml:math id="M1029" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, and biomass burning, which are not consistently captured across global chemistry models <xref ref-type="bibr" rid="bib1.bibx152 bib1.bibx79" id="paren.249"/>. Recent studies further suggest that tropospheric oxidative capacity is itself evolving over time: <xref ref-type="bibr" rid="bib1.bibx79" id="text.250"/> infer an increasing global OH abundance from radiocarbon monoxide <inline-formula><mml:math id="M1030" display="inline"><mml:mrow class="chem"><mml:msup><mml:mo>(</mml:mo><mml:mn mathvariant="normal">14</mml:mn></mml:msup><mml:mi mathvariant="normal">CO</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> observations, with implications for the interpretation of recent <inline-formula><mml:math id="M1031" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> trends <xref ref-type="bibr" rid="bib1.bibx21 bib1.bibx82" id="paren.251"/>. Satellite-based observations have also been explored as a means to better characterize tropospheric OH distributions and reduce these uncertainties <xref ref-type="bibr" rid="bib1.bibx94" id="paren.252"/>.</p>
      <p id="d2e15143">The sensitivity of simulated <inline-formula><mml:math id="M1032" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions to OH variability (Fig. <xref ref-type="fig" rid="F6"/>d) is relatively uniform globally, with an average SD of 49.6 <inline-formula><mml:math id="M1033" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> (RSD of 3.6 <inline-formula><mml:math id="M1034" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>). This confirms that the oxidative sink is a dominant factor controlling methane concentrations and that its uncertainties propagate broadly rather than being confined to specific regions <xref ref-type="bibr" rid="bib1.bibx152 bib1.bibx21 bib1.bibx4 bib1.bibx82 bib1.bibx125" id="paren.253"/>. While OH-related uncertainties propagate globally and uniformly, their impact near source regions appears limited (Fig. <xref ref-type="fig" rid="F6"/>d). This is particularly relevant given ongoing concerns about <inline-formula><mml:math id="M1035" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>–OH interactions in polluted areas, where local nonlinearities may arise due to complex dependencies of OH concentrations on emissions of <inline-formula><mml:math id="M1036" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>, CO, and volatile organic compounds (VOCs) <xref ref-type="bibr" rid="bib1.bibx62 bib1.bibx40 bib1.bibx43 bib1.bibx61 bib1.bibx36" id="paren.254"/>. In theory, elevated <inline-formula><mml:math id="M1037" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> concentrations could partially saturate the OH sink, especially in regions with high levels of co-emitted VOCs and <inline-formula><mml:math id="M1038" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mi>x</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> that alter oxidative capacity. However, this expected nonlinearity is not strongly expressed in the <inline-formula><mml:math id="M1039" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> sensitivity maps. Because OH concentrations are prescribed and do not respond to <inline-formula><mml:math id="M1040" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> levels in our configuration, the oxidative capacity is higher than it would be under interactive chemistry. This conservative setup further dampens any potential <inline-formula><mml:math id="M1041" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>–OH saturation effects, explaining the relatively uniform <inline-formula><mml:math id="M1042" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> sensitivity patterns shown in Fig. <xref ref-type="fig" rid="F6"/>d. Moreover, the SD induced by OH variability exceeds the observed SD of <inline-formula><mml:math id="M1043" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions at most monitoring sites, indicating that OH-related uncertainties alone can introduce model variability greater than observational noise.</p>
      <p id="d2e15286">Regarding the kinetic isotope effect, Figs. <xref ref-type="fig" rid="F6"/>f and  S5f in the Supplement show that uncertainties in the OH-KIE induce a geographically homogeneous SD of 0.4 <inline-formula><mml:math id="M1044" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (RSD of 2.2 <inline-formula><mml:math id="M1045" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) in the atmospheric <inline-formula><mml:math id="M1046" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1047" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1048" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal, exceeding the observed SD at surface stations <xref ref-type="bibr" rid="bib1.bibx75 bib1.bibx117" id="paren.255"/>. This sensitivity is driven by only two published experimental determinations of the <inline-formula><mml:math id="M1049" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">12</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow><mml:mo>/</mml:mo><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> KIE for <inline-formula><mml:math id="M1050" display="inline"><mml:mrow><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow><mml:mo>+</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">OH</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>: <xref ref-type="bibr" rid="bib1.bibx16" id="text.256"/> (<inline-formula><mml:math id="M1051" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.0054</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.0009</mml:mn></mml:mrow></mml:math></inline-formula> at 296 <inline-formula><mml:math id="M1052" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi></mml:mrow></mml:math></inline-formula>) and <xref ref-type="bibr" rid="bib1.bibx108" id="text.257"/> (<inline-formula><mml:math id="M1053" display="inline"><mml:mrow><mml:mn mathvariant="normal">1.0039</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.0004</mml:mn></mml:mrow></mml:math></inline-formula> at 296 <inline-formula><mml:math id="M1054" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi></mml:mrow></mml:math></inline-formula>). No measurements exist below 278 <inline-formula><mml:math id="M1055" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi></mml:mrow></mml:math></inline-formula>, although theoretical calculations suggest the KIE may increase at lower temperatures <xref ref-type="bibr" rid="bib1.bibx39" id="paren.258"/>. At steady state, <xref ref-type="bibr" rid="bib1.bibx33" id="text.259"/> showed that the 0.0015 difference between the two values yields a <inline-formula><mml:math id="M1056" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1.3</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1057" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> shift in atmospheric <inline-formula><mml:math id="M1058" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1059" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1060" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, illustrating the high leverage of this parameter. In practice, previous inversions have adopted either value, <xref ref-type="bibr" rid="bib1.bibx108" id="text.260"/> in e.g. <xref ref-type="bibr" rid="bib1.bibx83 bib1.bibx114 bib1.bibx3 bib1.bibx136" id="text.261"/>, and <xref ref-type="bibr" rid="bib1.bibx16" id="text.262"/> in e.g. <xref ref-type="bibr" rid="bib1.bibx102" id="text.263"/>. This choice is absorbed by the posterior source mixture. Accordingly, we recommend treating the full Cantrell–Saueressig range in inversion frameworks (see Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>).</p>
      <p id="d2e15504">Beyond OH, two additional sinks contribute to the <inline-formula><mml:math id="M1061" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1062" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1063" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> budget and deserve explicit discussion: oxidation by chlorine (Cl) and soil uptake. Both are included in our forward simulations (Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>) but were not perturbed in dedicated sensitivity experiments.</p>
      <p id="d2e15538">The Cl sink accounts for a small fraction of total <inline-formula><mml:math id="M1064" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> oxidation. Recent estimates converge on a tropospheric contribution of <inline-formula><mml:math id="M1065" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>–3 <inline-formula><mml:math id="M1066" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of the total chemical sink <xref ref-type="bibr" rid="bib1.bibx44 bib1.bibx121 bib1.bibx38 bib1.bibx145" id="paren.264"/>, with the latest Global Methane Budget reporting a climatological tropospheric Cl sink of <inline-formula><mml:math id="M1067" display="inline"><mml:mrow><mml:mn mathvariant="normal">6</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mo>[</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>–<inline-formula><mml:math id="M1068" display="inline"><mml:mrow><mml:mn mathvariant="normal">13</mml:mn><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1069" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx111" id="paren.265"/>, substantially smaller and better constrained than earlier estimates <xref ref-type="bibr" rid="bib1.bibx1" id="paren.266"/>. Despite this small magnitude, the Cl reaction carries an exceptionally large kinetic isotope effect (KIE <inline-formula><mml:math id="M1070" display="inline"><mml:mrow><mml:mo>≈</mml:mo><mml:mn mathvariant="normal">1.066</mml:mn></mml:mrow></mml:math></inline-formula> at 298 <inline-formula><mml:math id="M1071" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">K</mml:mi></mml:mrow></mml:math></inline-formula>; <xref ref-type="bibr" rid="bib1.bibx107" id="altparen.267"/>), more than an order of magnitude larger than that of OH, so even modest uncertainties in Cl concentrations translate into substantial shifts in modeled <inline-formula><mml:math id="M1072" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1073" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1074" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (see Table <xref ref-type="table" rid="T2"/>). <xref ref-type="bibr" rid="bib1.bibx3" id="text.268"/> further identified the combined uncertainty in fractionation (OH-KIE and Cl contribution) as the single most important factor limiting isotope-based source partitioning at the global scale <xref ref-type="bibr" rid="bib1.bibx105" id="paren.269"/>. <xref ref-type="bibr" rid="bib1.bibx135" id="text.270"/> quantified this influence within the same CIF-LMDz-SACS framework used here, and reported a near-linear sensitivity of <inline-formula><mml:math id="M1075" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">11.7</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1076" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M1077" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1.0</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1078" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> in the globally averaged source signature per 1000 <inline-formula><mml:math id="M1079" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">molec</mml:mi><mml:mo>.</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">m</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> increase in mean tropospheric Cl, with stratospheric Cl alone contributing a <inline-formula><mml:math id="M1080" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">0.30</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1081" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> surface enrichment via stratosphere–troposphere exchange and modifying the <inline-formula><mml:math id="M1082" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1083" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1084" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> seasonal cycle amplitude by up to 10 <inline-formula><mml:math id="M1085" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>–20 <inline-formula><mml:math id="M1086" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> depending on latitude. Because our configuration adopts the Cl field from <xref ref-type="bibr" rid="bib1.bibx145" id="text.271"/>, consistent with the most recent tropospheric chlorine chemistry, the Cl-related uncertainty in our simulations is bounded by the ranges quantified in <xref ref-type="bibr" rid="bib1.bibx135" id="text.272"/>, which are of the same order of magnitude as the OH-KIE sensitivity reported in Table <xref ref-type="table" rid="T6"/>. A dedicated Cl sensitivity experiment was therefore not repeated here to avoid duplicating a recent and comprehensive analysis with the same model.</p>
      <p id="d2e15836">Soil uptake contributes <inline-formula><mml:math id="M1087" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">31</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mo>[</mml:mo><mml:mn mathvariant="normal">17</mml:mn></mml:mrow></mml:math></inline-formula>–<inline-formula><mml:math id="M1088" display="inline"><mml:mrow><mml:mn mathvariant="normal">39</mml:mn><mml:mo>]</mml:mo></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1089" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> to the global <inline-formula><mml:math id="M1090" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> budget <xref ref-type="bibr" rid="bib1.bibx111" id="paren.273"/>, or about 5 <inline-formula><mml:math id="M1091" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of the total <inline-formula><mml:math id="M1092" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> sink, with a moderate KIE of <inline-formula><mml:math id="M1093" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1.020</mml:mn></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx126" id="paren.274"/>, intermediate between OH (1.0039) and Cl (1.066) (see Table <xref ref-type="table" rid="T2"/>). In our framework, it is implemented as a first-order deposition process with isotope-dependent deposition velocities (Sect. <xref ref-type="sec" rid="Ch1.S3.SS1.SSS5"/>). Given its small relative contribution to the total sink, its moderate KIE, and the well-constrained global magnitude reported in recent budgets, soil uptake uncertainties are expected to have a substantially smaller impact on the modeled <inline-formula><mml:math id="M1094" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1095" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1096" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal than the OH-KIE (Table <xref ref-type="table" rid="T6"/>), and were therefore not perturbed in the Monte Carlo ensemble.</p>
      <p id="d2e15970">In summary, OH-KIE is the dominant chemistry-related driver of <inline-formula><mml:math id="M1097" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1098" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1099" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> variability, while OH fields dominate <inline-formula><mml:math id="M1100" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction sensitivity. The Cl sink also exerts a strong leverage on <inline-formula><mml:math id="M1101" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1102" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1103" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> through its large KIE; its impact within the same CIF-LMDz-SACS framework has been comprehensively quantified by <xref ref-type="bibr" rid="bib1.bibx135" id="text.275"/> and is therefore not duplicated here.</p>
</sec>
<sec id="Ch1.S4.SS2.SSS4">
  <label>4.2.4</label><title>Sensitivity of simulated atmospheric <inline-formula><mml:math id="M1104" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1105" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1106" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> to source signatures</title>
      <p id="d2e16084">Figures <xref ref-type="fig" rid="F7"/> and S8 in the Supplement present the sensitivity of the simulated atmospheric <inline-formula><mml:math id="M1107" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1108" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1109" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal to uncertainties in source-specific isotopic signatures, based on the Monte Carlo simulations (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>). Panel (a) displays the SD of the prescribed <inline-formula><mml:math id="M1110" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1111" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1112" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures used as input to the simulations. The highest signature RSDs are associated with the BB sector, with an RSD of 36 <inline-formula><mml:math id="M1113" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> and a SD of 7.8 <inline-formula><mml:math id="M1114" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>,  followed by FFG sector (RSD: 13.0 <inline-formula><mml:math id="M1115" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>, SD: 6.1 <inline-formula><mml:math id="M1116" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), NAT sector (RSD: 12.0 <inline-formula><mml:math id="M1117" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>, SD: 5.3 <inline-formula><mml:math id="M1118" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), WET sector (RSD: 9.2 <inline-formula><mml:math id="M1119" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>, SD: 5.2 <inline-formula><mml:math id="M1120" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), and AGW sector (RSD: 7.3 <inline-formula><mml:math id="M1121" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>, SD: 4.6 <inline-formula><mml:math id="M1122" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). These RSD values are consistent with the sector-specific uncertainty ranges summarized in Table S3. The spatial pattern of these uncertainties reflects the regional sampling domains used in the Monte Carlo parameterization (see Sect. <xref ref-type="sec" rid="Ch1.S3.SS2"/>).</p>

      <fig id="F7" specific-use="star"><label>Figure 7</label><caption><p id="d2e16236"><bold>(a)</bold> SD (in <inline-formula><mml:math id="M1123" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) of the <inline-formula><mml:math id="M1124" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1125" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1126" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature sensitivities inputs for Monte Carlo simulations, by sector at surface level. <bold>(b)</bold> SD of the <inline-formula><mml:math id="M1127" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1128" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1129" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signal from Monte Carlo simulations, by sector at surface level. Coloured circles indicate RSD of observed <inline-formula><mml:math id="M1130" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1131" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1132" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> values at each surface station over the study period <xref ref-type="bibr" rid="bib1.bibx75 bib1.bibx117" id="paren.276"/>.</p></caption>
            <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f07.png"/>

          </fig>

      <p id="d2e16349">Panel (b) shows the resulting variability in modeled atmospheric <inline-formula><mml:math id="M1133" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1134" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1135" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>  at surface level. These simulations only perturb the isotopic composition of the emissions while keeping total <inline-formula><mml:math id="M1136" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> fluxes fixed, as a result, there is no corresponding effect on <inline-formula><mml:math id="M1137" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions. Despite having a comparatively lower SD in its source signature, the AGW sector emerges as the dominant driver of atmospheric <inline-formula><mml:math id="M1138" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1139" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1140" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> uncertainty, with a mean sensitivity of 0.32 <inline-formula><mml:math id="M1141" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (1.74 <inline-formula><mml:math id="M1142" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>). This impact is particularly pronounced in regions with high AGW emissions, such as India, where EDGARv8 estimates an annual mean emission of 26 <inline-formula><mml:math id="M1143" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> per year over the period 2016–2020. Other sectors contribute less significantly to overall isotopic variability but still have regionally relevant effects: BB contributes 0.16 <inline-formula><mml:math id="M1144" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (0.84 <inline-formula><mml:math id="M1145" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), FFG 0.04 <inline-formula><mml:math id="M1146" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (0.43 <inline-formula><mml:math id="M1147" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), NAT 0.07 <inline-formula><mml:math id="M1148" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (0.38 <inline-formula><mml:math id="M1149" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>), and WET 0.02 <inline-formula><mml:math id="M1150" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (0.10 <inline-formula><mml:math id="M1151" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>).</p>
      <p id="d2e16530">Uncertainties in source-specific isotopic signatures, particularly from AGW sector, translate into substantial variability in the simulated <inline-formula><mml:math id="M1152" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1153" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1154" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal. This effect is especially pronounced in emission hotspots, where even small shifts in isotopic assumptions can significantly affect local atmospheric signals. Conversely, background regions remain sensitive to these uncertainties through long-range transport, potentially biasing hemispheric or global source attribution. Moreover, the mean RSD induced by AGW source signature uncertainties (1.74 <inline-formula><mml:math id="M1155" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula>) exceeds the observed RSD of <inline-formula><mml:math id="M1156" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1157" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1158" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> at most surface stations, suggesting that this parameter is a major limiting factor for isotopic inversions. For other sectors (e.g. BB, FFG, NAT), the simulated RSD remains generally closer to or below observed values, depending on the station location and the local sensitivity to each source's isotopic signature. These findings underscore the need to improve isotopic characterization of agricultural and waste-related methane sources, especially in hotspots regions. Implications for the design and configuration of such systems are discussed in Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>.</p>
      <p id="d2e16602">In summary, AGW source signature uncertainties dominate isotopic variability despite a moderate input SD, due to the large flux of this sector. BB, FFG, NAT and WET signature uncertainties have comparatively limited atmospheric impact at the global scale but produce regionally important effects. Improving AGW isotopic characterization, particularly in emission hotspots, is the highest-priority lever for source-signature-related uncertainty reduction.</p>
      <p id="d2e16605">Our sensitivity analysis shows that uncertainties in the OH kinetic isotope effect (KIE) are the dominant drivers of variability in the modeled <inline-formula><mml:math id="M1159" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1160" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1161" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal at global scale. Uncertainties in agriculture and waste sector source signatures and fluxes also contribute significantly. In contrast, uncertainties associated with fossil fuel and wetland source signatures, as well as those related to fluxes used for aggregation, have a more limited impact at the global level (more details in Sect <xref ref-type="sec" rid="Ch1.S4.SS3.SSS1"/>).</p>
</sec>
</sec>
<sec id="Ch1.S4.SS3">
  <label>4.3</label><title>Discussion</title>
      <p id="d2e16648">This section discusses the key outcomes of the sensitivity analysis (Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS1"/>) and their implications for atmospheric methane inversions (Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>). We examine how the sensitivity analysis results can inform the configuration of isotopic inversions, particularly regarding uncertainty specification and parameter prioritization. The main objective is to distinguish between uncertainty components that could be reduced through improved input data or model structure, and those that are intrinsic and must be explicitly optimized within the inversion framework (see Fig. <xref ref-type="fig" rid="F4"/>). Finally, we identify opportunities for future improvements, both within inversion systems and through supporting efforts such as inventories, field campaigns, and process-based models (Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS3"/>).</p>
<sec id="Ch1.S4.SS3.SSS1">
  <label>4.3.1</label><title>Key uncertainty drivers affecting <inline-formula><mml:math id="M1162" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M1163" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1164" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1165" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> simulations</title>
      <p id="d2e16707">This section synthesizes the sensitivity results presented in Sect. <xref ref-type="sec" rid="Ch1.S4.SS2"/> and identifies the dominant drivers of uncertainty in modeled <inline-formula><mml:math id="M1166" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions and <inline-formula><mml:math id="M1167" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1168" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1169" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signals. Figure <xref ref-type="fig" rid="F8"/> provides an integrated overview, locating each tested parameter according to its joint impact on both quantities. Parameters in the upper-right quadrant induce the largest uncertainties simultaneously in <inline-formula><mml:math id="M1170" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M1171" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1172" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1173" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and therefore represent priority targets for model improvement. As detailed in Sect. <xref ref-type="sec" rid="Ch1.S4.SS2"/>, freshwater fluxes and OH fields dominate <inline-formula><mml:math id="M1174" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> variability, while OH-KIE and AGW source signatures dominate <inline-formula><mml:math id="M1175" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1176" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1177" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> variability. Aggregation choices, as well as FFG, BB, NAT and WET source signatures, exert a comparatively limited influence at the global scale. These findings are consistent with previous work identifying OH-KIE as a primary limitation for isotopic source partitioning  <xref ref-type="bibr" rid="bib1.bibx3 bib1.bibx17" id="paren.277"/>, and extend earlier analyses by quantifying the additional contribution of interannual variability in OH fields, wetland and freshwater fluxes, and isotopic source signatures.</p>

      <fig id="F8" specific-use="star"><label>Figure 8</label><caption><p id="d2e16843">Uncertainties in <inline-formula><mml:math id="M1178" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction and the <inline-formula><mml:math id="M1179" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1180" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1181" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> isotopic signal across various parameters. The <inline-formula><mml:math id="M1182" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis shows the SD of <inline-formula><mml:math id="M1183" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions in parts per billion <inline-formula><mml:math id="M1184" display="inline"><mml:mrow class="unit"><mml:mo>(</mml:mo><mml:mi mathvariant="normal">ppb</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, while the <inline-formula><mml:math id="M1185" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axis shows the SD of the <inline-formula><mml:math id="M1186" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1187" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1188" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal in per mil (<inline-formula><mml:math id="M1189" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). Each point represents a simulated grid cell, and the point labeled <italic>OBS</italic> corresponds to observations from a surface monitoring station. Parameters located in the upper-right quadrant induce the largest uncertainties in both mole fraction and isotopic composition.</p></caption>
            <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f08.png"/>

          </fig>

      <p id="d2e16971">To assess whether these modeled sensitivities are large enough to matter for inversion frameworks, they must be compared to the natural variability captured by atmospheric observations. The observed standard deviation of surface <inline-formula><mml:math id="M1190" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fractions reaches 44 <inline-formula><mml:math id="M1191" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula>, while that of <inline-formula><mml:math id="M1192" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1193" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1194" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is 0.23 <inline-formula><mml:math id="M1195" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> (Fig. S8). Several parameters tested here exceed these thresholds: freshwater fluxes and OH fields for <inline-formula><mml:math id="M1196" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, and OH-KIE, AGW source signatures and wetland fluxes for <inline-formula><mml:math id="M1197" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1198" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1199" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. This means that the uncertainties associated with these parameters are not absorbed by observational noise and propagate directly into inversion outcomes. The magnitude of these uncertainties is also non-negligible relative to the long-term atmospheric trends used to interpret methane budget changes, namely <inline-formula><mml:math id="M1200" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">9.4</mml:mn><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.3</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1201" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi><mml:mspace width="0.125em" linebreak="nobreak"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for <inline-formula><mml:math id="M1202" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> over 2016–2020 <xref ref-type="bibr" rid="bib1.bibx57" id="paren.278"/> and approximately <inline-formula><mml:math id="M1203" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">0.04</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1204" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> for <inline-formula><mml:math id="M1205" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1206" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1207" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx117" id="paren.279"/>, reinforcing the need for explicit treatment in inversion configurations.</p>
      <p id="d2e17179">Figure <xref ref-type="fig" rid="F9"/> illustrates the spatial distribution of the dominant source of uncertainty in each grid cell, complemented by Fig. S9 and S10 in the Supplement which provide a detailed quantification of the contribution of each parameter to the total variance of the simulated <inline-formula><mml:math id="M1208" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1209" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1210" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal and <inline-formula><mml:math id="M1211" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction at the model grid cell level. Beyond globally aggregated diagnostics, this spatial classification reveals a strongly heterogeneous structure, with OH-KIE dominating <inline-formula><mml:math id="M1212" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1213" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1214" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> variance over most of the globe (around 50 <inline-formula><mml:math id="M1215" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of total variance) and regional exceptions emerging in well-defined emission hotspots. Four regional case studies illustrate the diversity of dominant drivers and provide context for the targeted improvements discussed in Sects. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/> and <xref ref-type="sec" rid="Ch1.S4.SS3.SSS3"/>. <list list-type="bullet"><list-item>
      <p id="d2e17268">Indo-Gangetic Plain: AGW source signatures contribute up to 80 <inline-formula><mml:math id="M1216" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of the local <inline-formula><mml:math id="M1217" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1218" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1219" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> variance over this region. This dominance reflects both the magnitude of regional AGW emissions (<inline-formula><mml:math id="M1220" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">26</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1221" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Tg</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msup><mml:mi mathvariant="normal">yr</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula> from EDGARv8 over 2016–2020) and the strong isotopic contrast between livestock (<inline-formula><mml:math id="M1222" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">65.8</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1223" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>) and waste sub-sectors (<inline-formula><mml:math id="M1224" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">50.9</mml:mn></mml:mrow></mml:math></inline-formula> to <inline-formula><mml:math id="M1225" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">56.2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1226" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). The relative livestock share varies from 67 <inline-formula><mml:math id="M1227" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> (EDGARv8) to 79 <inline-formula><mml:math id="M1228" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> (CEDS, GAINS), directly generating the spread observed in atmospheric simulations. Resolving this hotspot requires improved partitioning between livestock and waste sub-sectors in regional inventories, complemented by isotopic measurements that capture <inline-formula><mml:math id="M1229" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula><inline-formula><mml:math id="M1230" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula><inline-formula><mml:math id="M1231" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> dietary heterogeneity. The Ethiopian highlands provide a finer-scale illustration of this need: the <inline-formula><mml:math id="M1232" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula><inline-formula><mml:math id="M1233" display="inline"><mml:mo>/</mml:mo></mml:math></inline-formula><inline-formula><mml:math id="M1234" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> forage balance varies with altitude, producing sub-national contrasts in livestock signatures <xref ref-type="bibr" rid="bib1.bibx13" id="paren.280"/> that current global inventories cannot resolve. Emerging evidence from dual-isotope (<inline-formula><mml:math id="M1235" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1236" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>–<inline-formula><mml:math id="M1237" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1238" display="inline"><mml:mrow class="chem"><mml:mi mathvariant="normal">D</mml:mi></mml:mrow></mml:math></inline-formula>) measurements over South Asia <xref ref-type="bibr" rid="bib1.bibx150" id="paren.281"><named-content content-type="pre">e.g.</named-content></xref> suggests that AGW emissions in this region may carry distinct isotopic fingerprints from co-located fossil fuel sources, supporting the use of multi-isotopic constraints for source disentanglement in densely emitting tropical regions.</p></list-item><list-item>
      <p id="d2e17501">Tropical wetlands (Congo Basin, Amazon, Borneo): Wetland flux uncertainties dominate over these regions, reaching more than 60 <inline-formula><mml:math id="M1239" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of local <inline-formula><mml:math id="M1240" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1241" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1242" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> variance in Borneo. These regions host some of the largest global wetland emissions but remain critically under-sampled. Recent tropical airborne and ground-based campaigns <xref ref-type="bibr" rid="bib1.bibx32 bib1.bibx86 bib1.bibx120" id="paren.282"/> have begun addressing this gap, reporting signatures broadly consistent with those used here but covering only a limited number of sites. Sustained measurement programs in these basins are essential to constrain both flux magnitudes and isotopic signatures of tropical wetland emissions.</p></list-item><list-item>
      <p id="d2e17545">Caspian region: Freshwater flux uncertainties account for more than 60 <inline-formula><mml:math id="M1243" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">%</mml:mi></mml:mrow></mml:math></inline-formula> of the local <inline-formula><mml:math id="M1244" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1245" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1246" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> variance. The Caspian Sea is a large endorheic brackish lake, treated here as a freshwater source given the absence of a dedicated dataset for endorheic systems; this classification ambiguity, combined with proximity to major oil and gas infrastructure in Turkmenistan and Azerbaijan, makes regional source attribution particularly challenging. More broadly, freshwater emissions remain poorly constrained due to complex emission pathways and limited mapping of inland water extent <xref ref-type="bibr" rid="bib1.bibx59 bib1.bibx111" id="paren.283"/>.</p></list-item></list></p>

      <fig id="F9" specific-use="star"><label>Figure 9</label><caption><p id="d2e17590">Spatial distribution of the dominant uncertainty driver (parameter with the highest RSD) in each grid cell at the surface. The second row of plots shows the dominant uncertainty category after removing the primary driver from the analysis. Surface stations are indicated with black dots.</p></caption>
            <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f09.png"/>

          </fig>

      <p id="d2e17599">The second row of Fig. <xref ref-type="fig" rid="F9"/> highlights the secondary drivers that would emerge if first-order uncertainties were reduced, with anthropogenic and freshwater fluxes becoming critical in many additional regions. Together, these case studies support a key conceptual distinction between two regimes of uncertainty: localized hotspots, where large uncertainties hinder source attribution at the regional scale and where targeted external efforts (inventories, field campaigns, process models) can reduce prior errors; and remote or well-mixed background regions, where uncertainties are dominated by OH-KIE and propagate through long-range transport, requiring explicit optimization within the inversion framework. The implications of this distinction for inversion design, including <inline-formula><mml:math id="M1247" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M1248" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> matrix specification, are detailed in Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS2"/>.</p>
</sec>
<sec id="Ch1.S4.SS3.SSS2">
  <label>4.3.2</label><title>Implications for isotopic inversions</title>
      <p id="d2e17628">The sensitivity results synthesized in Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS1"/> directly inform the design of isotopic inversions. The central question is how to allocate effort between two complementary strategies: reducing prior uncertainties through external inputs (inventories, process models, field campaigns), and explicitly optimizing intrinsic uncertainties within the inversion framework. <xref ref-type="bibr" rid="bib1.bibx135" id="text.284"/> previously emphasized the need for spatially explicit, sectorally disaggregated uncertainty assessments to guide this allocation, and the present study fills this gap through an ensemble of forward simulations.</p>
      <p id="d2e17636">Reducible uncertainties primarily concern AGW source signatures, freshwater fluxes, and wetland fluxes, which dominate in localized hotspots (Sect. <xref ref-type="sec" rid="Ch1.S4.SS3.SSS1"/>). They can be addressed through external efforts complementary to inversion development: expanded inventories with finer spatial and sectoral resolution, dedicated isotopic field campaigns, and refined process-based models. The risk of co-located sources with overlapping signatures, previously highlighted by <xref ref-type="bibr" rid="bib1.bibx25" id="text.285"/>, reinforces the need for these external efforts: without them, unresolved prior uncertainties propagate into the inversion and lead to ambiguous source attribution (Fig. <xref ref-type="fig" rid="F4"/>).</p>
      <p id="d2e17646">Intrinsic uncertainties, primarily related to the OH-KIE, cannot be reduced through prior refinement and must instead be sampled within the inversion framework via ensemble-based or variational approaches, unless laboratory or theoretical advances narrow the Cantrell–Saueressig range. This recommendation aligns with <xref ref-type="bibr" rid="bib1.bibx55" id="text.286"/> and addresses a gap identified by <xref ref-type="bibr" rid="bib1.bibx3" id="text.287"/> and <xref ref-type="bibr" rid="bib1.bibx136" id="text.288"/>, namely the lack of robust, data-driven uncertainty estimates for source signatures and KIE in current <inline-formula><mml:math id="M1249" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1250" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1251" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> inversions.</p>
      <p id="d2e17687">The sectoral total uncertainties <inline-formula><mml:math id="M1252" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>total</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> reported in Table <xref ref-type="table" rid="T4"/> provide a quantitative basis for specifying the diagonal terms of the prior error covariance matrix <inline-formula><mml:math id="M1253" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula>. The sensitivity ranges quantified in Sect. <xref ref-type="sec" rid="Ch1.S4.SS2"/> similarly inform the model–observation mismatch component of the observation error matrix <inline-formula><mml:math id="M1254" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> when source signatures or KIE are held fixed. The relative magnitude of <inline-formula><mml:math id="M1255" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M1256" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> determines whether each parameter can be effectively constrained: when <inline-formula><mml:math id="M1257" display="inline"><mml:mrow><mml:mi mathvariant="bold">B</mml:mi><mml:mo>≫</mml:mo><mml:mi mathvariant="bold">R</mml:mi></mml:mrow></mml:math></inline-formula> and the parameter has a detectable atmospheric signature, the inversion reduces uncertainty significantly; when <inline-formula><mml:math id="M1258" display="inline"><mml:mrow><mml:mi mathvariant="bold">B</mml:mi><mml:mo>≪</mml:mo><mml:mi mathvariant="bold">R</mml:mi></mml:mrow></mml:math></inline-formula>, the posterior remains close to the prior. These relationships, schematized in Fig. <xref ref-type="fig" rid="F4"/> and extended to the isotopic case in Fig. <xref ref-type="fig" rid="F10"/>, provide the rationale for the configuration choices recommended below. Where observations are sparse, particularly in the Southern Hemisphere, spatial clustering based on isotopic similarity may improve inversion stability.</p>

      <fig id="F10" specific-use="star"><label>Figure 10</label><caption><p id="d2e17765">Schematic illustration of the effect of adding <inline-formula><mml:math id="M1259" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1260" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1261" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> constraints in the inversion. The upper panel shows the reference case using <inline-formula><mml:math id="M1262" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> only, where co-located emissions are difficult to disentangle. The middle panel illustrates the case where <inline-formula><mml:math id="M1263" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1264" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1265" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures are fixed with no uncertainty (<inline-formula><mml:math id="M1266" display="inline"><mml:mrow><mml:mi mathvariant="bold">B</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:math></inline-formula>), which provides a strong constraint but may lead to potential biases if the signatures are mis-specified. The lower panel shows the case where <inline-formula><mml:math id="M1267" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1268" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1269" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures are optimized with realistic uncertainties, which improves the ability to disentangle emission sectors but requires a careful balance between  <inline-formula><mml:math id="M1270" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula> and  <inline-formula><mml:math id="M1271" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> to avoid ineffective constraints. Coloured Gaussian curves represent prior, observational and posterior distributions for <inline-formula><mml:math id="M1272" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> fluxes and <inline-formula><mml:math id="M1273" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1274" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1275" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures, with the forward model <inline-formula><mml:math id="M1276" display="inline"><mml:mrow><mml:mi mathvariant="script">H</mml:mi><mml:mo>(</mml:mo><mml:mi>x</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> linking the parameter space to the observation space.</p></caption>
            <graphic xlink:href="https://essd.copernicus.org/articles/18/4793/2026/essd-18-4793-2026-f10.png"/>

          </fig>

      <p id="d2e17954">Several practical recommendations emerge from this framework: <list list-type="bullet"><list-item>
      <p id="d2e17959">AGW sectoral granularity: Within the AGW sector, livestock and waste sub-sectors carry strongly contrasted signatures (Table <xref ref-type="table" rid="T1"/>) and should not be merged into a single category, in agreement with <xref ref-type="bibr" rid="bib1.bibx73" id="text.289"/> and <xref ref-type="bibr" rid="bib1.bibx67" id="text.290"/>. The five sub-sector structure used here is sufficient at the global scale (Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS1"/>, NO_AGGREG test), but the livestock–waste distinction must be preserved in inversion priors. Within this five sub-sector structure, the dominant AGW contribution to atmospheric <inline-formula><mml:math id="M1277" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1278" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1279" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> uncertainty (Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS4"/>, Table <xref ref-type="table" rid="T6"/>) originates from uncertainty on the sub-sector signature values themselves, not from how they are aggregated; this should guide the specification of the prior error covariance matrix for AGW signatures.</p>
      <p id="d2e18006">Freshwater treatment: Freshwater fluxes have a strong <inline-formula><mml:math id="M1280" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signature but remain poorly constrained. Including them within an extended wetland category, rather than as a separate optimized source, may currently offer the best trade-off until more observational data become available. Omitting them entirely would bias regional attribution, particularly in Central Asia and the tropics.</p></list-item><list-item>
      <p id="d2e18021">OH treatment: Although OH does not affect <inline-formula><mml:math id="M1281" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1282" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1283" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> directly, it propagates strongly into <inline-formula><mml:math id="M1284" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction variability and should be incorporated through chemistry ensemble fields rather than fixed climatologies.</p></list-item><list-item>
      <p id="d2e18065">Aggregation transferability: The minor sensitivity to aggregation choices (Sect. <xref ref-type="sec" rid="Ch1.S4.SS2.SSS1"/>) supports the use of the isotopic maps developed here across diverse inversion systems and emission inventories, provided sub-sector heterogeneity within AGW is preserved.</p></list-item></list></p>
      <p id="d2e18070">These recommendations build on and quantify the qualitative needs identified by <xref ref-type="bibr" rid="bib1.bibx3" id="text.291"/> and <xref ref-type="bibr" rid="bib1.bibx136" id="text.292"/>, and provide a directly usable basis for configuring the next generation of <inline-formula><mml:math id="M1285" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1286" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1287" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> inversions.</p>
</sec>
<sec id="Ch1.S4.SS3.SSS3">
  <label>4.3.3</label><title>Pathways for improvement</title>
      <p id="d2e18116">Beyond the inversion configuration choices discussed in Sect. 4.3.2, several research directions are needed to reduce the uncertainties identified in this study. These cut across three complementary axes: temporal representativeness of source signatures, atmospheric transport and chemistry, and process-level understanding of natural emissions.</p>
      <p id="d2e18119">A first priority concerns the temporal dimension of isotopic signatures, which is currently held constant for most sub-sectors over 1998–2022. Documented changes in livestock feeding practices, particularly the evolving balance between <inline-formula><mml:math id="M1288" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M1289" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> plant diets, are known to modulate ruminant <inline-formula><mml:math id="M1290" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1291" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1292" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signatures <xref ref-type="bibr" rid="bib1.bibx18 bib1.bibx55" id="paren.293"/> and remain insufficiently represented. Similarly, finer differentiation between waste sub-sectors (landfills, wastewater, agricultural waste) would improve AGW characterization <xref ref-type="bibr" rid="bib1.bibx73" id="paren.294"/>. Because seasonal variations in <inline-formula><mml:math id="M1293" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1294" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1295" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> are particularly sensitive to small shifts in source signatures, both their amplitude and phase can be affected <xref ref-type="bibr" rid="bib1.bibx50" id="paren.295"/>, making temporal characterization a critical lever for inversion performance.</p>
      <p id="d2e18212">A second priority concerns atmospheric transport and chemistry, which were not perturbed in our sensitivity ensemble. All simulations were performed with LMDz at a single resolution (Sect. <xref ref-type="sec" rid="Ch1.S3.SS1.SSS1"/>), and the TransCom-<inline-formula><mml:math id="M1296" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> intercomparison <xref ref-type="bibr" rid="bib1.bibx92" id="paren.296"/> showed that modeled <inline-formula><mml:math id="M1297" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> budgets are sensitive to troposphere–stratosphere exchange rates and to vertical grid structure, with <inline-formula><mml:math id="M1298" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> lifetimes spanning 9.50–10.27 <inline-formula><mml:math id="M1299" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">yr</mml:mi></mml:mrow></mml:math></inline-formula> across 12 CTMs using identical OH fields. For <inline-formula><mml:math id="M1300" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1301" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1302" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, vertical transport additionally controls the rate at which <inline-formula><mml:math id="M1303" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-enriched stratospheric air re-enters the troposphere via the Brewer–Dobson circulation, as well as the vertical distribution of the Cl sink and its strong fractionation <xref ref-type="bibr" rid="bib1.bibx14 bib1.bibx135" id="paren.297"/>. The sensitivity hierarchy identified here, dominated by OH-KIE and AGW signatures, is driven by prescribed inputs and is expected to be robust across CTMs, but quantifying transport-related uncertainty through multi-model ensembles remains a priority. In parallel, additional oxidation pathways deserve dedicated attention: emerging evidence for previously unaccounted-for Cl sources, notably photocatalytic release from mineral dust–sea spray aerosol <xref ref-type="bibr" rid="bib1.bibx142 bib1.bibx105" id="paren.298"/>, and the potential of novel tracers such as <inline-formula><mml:math id="M1304" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1305" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-CO to detect regional Cl-driven oxidation, should be considered in future isotopic inversion setups.</p>
      <p id="d2e18328">A third priority concerns process-level understanding of natural emissions. Wetland and freshwater methane emission models suffer from limited data on hydrological dynamics, organic matter content, and microbial population dynamics, particularly in tropical regions where the largest emissions coincide with the sparsest observations. Coordinated airborne and ground-based campaigns, exemplified by MOYA and ZWAMPS in tropical wetlands, rice fields, and biomass burning regions <xref ref-type="bibr" rid="bib1.bibx86 bib1.bibx32" id="paren.299"/>, provide a model for the type of effort needed to fill these observational gaps. Enhanced national reporting of sectoral emissions, particularly for waste and agriculture, and site-specific isotopic measurements in major fossil production basins and under-sampled freshwater systems are equally needed to constrain prior fluxes and signatures.</p>
      <p id="d2e18335">Together, these three axes define a research agenda complementary to inversion development itself: without parallel progress on temporal characterization, transport and chemistry, and process-based understanding, isotopic inversions will remain limited by the very priors they aim to constrain.</p>
</sec>
</sec>
</sec>
<sec id="Ch1.S5">
  <label>5</label><title>Code and data availability</title>
      <p id="d2e18349">Isotopic source signature datasets were provided by Xin Lan, Malika Menoud, Youmi Oh, and Giuseppe Etiope. The gridded <inline-formula><mml:math id="M1306" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1307" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1308" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature dataset (1998–2022) developed in this study is openly available under CC BY 4.0 at the ESA Open Science Data portal (<xref ref-type="bibr" rid="bib1.bibx133" id="altparen.300"/>,  <ext-link xlink:href="https://doi.org/10.57780/ESA-6D202E9" ext-link-type="DOI">10.57780/ESA-6D202E9</ext-link>). The atmospheric modeling framework used for the sensitivity analysis is based on the Community Inversion Framework (CIF; <xref ref-type="bibr" rid="bib1.bibx5" id="altparen.301"/>,  <ext-link xlink:href="https://doi.org/10.5194/gmd-14-5331-2021" ext-link-type="DOI">10.5194/gmd-14-5331-2021</ext-link>) coupled to the LMDz transport model. The dataset is provided at two levels of sectoral granularity to accommodate different modeling needs. The aggregated product contains gridded monthly <inline-formula><mml:math id="M1309" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1310" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1311" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signature maps for the five main source sectors used throughout this study (FFG, AGW, BB, WET, NAT). In addition, the disaggregated product provides gridded monthly <inline-formula><mml:math id="M1312" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1313" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1314" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signature maps for each of the 13 underlying sub-sectors (coal, oil and gas, geological, livestock, wastewater, landfills, agricultural waste, rice, biofuel burning, biomass burning, wetlands, termites, oceans). Users can therefore re-aggregate the dataset using their own sectoral classification or their preferred flux inventory, in line with the framework described in here. Scripts used for dataset processing and uncertainty analysis are available upon request from the corresponding author.</p>
</sec>
<sec id="Ch1.S6" sec-type="conclusions">
  <label>6</label><title>Conclusions</title>
      <p id="d2e18460">Existing global <inline-formula><mml:math id="M1315" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1316" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1317" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> datasets <xref ref-type="bibr" rid="bib1.bibx55 bib1.bibx89 bib1.bibx73 bib1.bibx136" id="paren.302"><named-content content-type="pre">e.g.</named-content></xref> have provided valuable benchmarks but were limited in temporal coverage, systematic uncertainty quantification, and compatibility with inversion-ready sectoral structures. To address these limitations, we produced an updated global dataset of <inline-formula><mml:math id="M1318" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1319" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1320" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signatures for five major natural and anthropogenic sectors, following the Global Methane Budget (GMB) classification. This aggregation strategy reduces the number of categories for computational efficiency in future inversion studies while preserving isotopic representativeness across emission types. The maps cover the period 1998–2022 and integrate recent spatially explicit datasets and literature-derived observations, providing explicit estimates of both intrinsic (within-sector) and aggregation-related uncertainties. Overall, this new dataset offers a temporally extended, uncertainty-quantified, and inversion-ready basis for atmospheric modeling and isotopic inversions. To support a broad range of inversion configurations, the dataset is distributed at two levels of sectoral granularity: the five-sector aggregated product used in this study, and the underlying 14 sub-sector maps, allowing users to re-aggregate according to their own classification or flux-weighting scheme.</p>
      <p id="d2e18527">Using forward simulations in the Community Inversion Framework coupled to the LMDz transport model, we conducted a comprehensive sensitivity analysis to assess the influence of key parameters on the modeled atmospheric <inline-formula><mml:math id="M1321" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1322" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1323" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal and <inline-formula><mml:math id="M1324" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mole fraction. Our results highlight that uncertainties in methane oxidation chemistry, particularly related to the OH kinetic isotope effect (KIE), and uncertainties in isotopic source signatures, especially from the agriculture and waste (AGW) sector, have the largest impact on the simulated isotopic ratios. By contrast, uncertainties related to flux aggregation, fossil fuel (FFG), wetland (WET) and other natural (NAT) isotopic source signatures have a more limited influence on global atmospheric signals.</p>
      <p id="d2e18570">We showed that isotopic uncertainties within certain sectors, such as the AGW sector (up to <inline-formula><mml:math id="M1325" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1326" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>), were substantial when compared to the standard deviation of atmospheric <inline-formula><mml:math id="M1327" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1328" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1329" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> observations at surface stations (approximately <inline-formula><mml:math id="M1330" display="inline"><mml:mrow><mml:mo>±</mml:mo><mml:mn mathvariant="normal">0.2</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1331" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula>). This emphasizes the importance of reducing uncertainties in source-specific signatures and isotopic fractionation processes to improve the reliability of atmospheric inversions.</p>
      <p id="d2e18639">Our results demonstrated the robustness of the proposed sector aggregation approach and confirmed the applicability of the updated isotopic maps across diverse inversion configurations. We recommend prioritizing efforts to better constrain isotopic signatures in the agriculture and waste sector, and to refine the OH kinetic isotope effect. Moreover, the methodology presented here for quantifying sectoral <inline-formula><mml:math id="M1332" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1333" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1334" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> uncertainties can be applied to future datasets as new observations become available, allowing the isotopic maps to be updated and the associated uncertainties reduced. In addition, we provide practical guidelines for configuring isotopic inversions, including recommended uncertainty ranges, key parameters to target for enhanced source attribution, and the use of regional optimization strategies in areas where uncertainties are most significant. The sectoral uncertainty estimates provided here can directly inform the specification of prior error covariance matrices in atmospheric inversion frameworks, thereby improving the consistency between sensitivity analyses and inversion configurations.</p>
      <p id="d2e18672">This study focused on developing and evaluating updated <inline-formula><mml:math id="M1335" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1336" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula>-<inline-formula><mml:math id="M1337" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> source signature maps through comparison with the literature, uncertainty quantification, and forward simulations. While direct validation using atmospheric data is beyond the scope of this paper, all necessary elements are provided, including gridded maps, uncertainty ranges, and sectoral breakdowns, to enable their integration into forward modeling and atmospheric inversions under optimal conditions.</p>
      <p id="d2e18704">Finally, the increasing availability of satellite-based <inline-formula><mml:math id="M1338" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and isotopic measurements opens promising perspectives for constraining methane sources at the global scale. Feasibility studies <xref ref-type="bibr" rid="bib1.bibx65 bib1.bibx66" id="paren.303"/> have shown that instruments such as GOSAT-2, TROPOMI, and Sentinel-5/UVNS could in principle retrieve <inline-formula><mml:math id="M1339" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, but several technical limitations currently prevent routine isotopic retrievals. Individual <inline-formula><mml:math id="M1340" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> retrieval uncertainties remain large: <xref ref-type="bibr" rid="bib1.bibx66" id="text.304"/> report mean uncertainties of <inline-formula><mml:math id="M1341" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1342" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> for TROPOMI (SWIR3 channel) and <inline-formula><mml:math id="M1343" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.68</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1344" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> for Sentinel-5/UVNS (SWIR1 channel), whereas the target <inline-formula><mml:math id="M1345" display="inline"><mml:mi mathvariant="italic">δ</mml:mi></mml:math></inline-formula><inline-formula><mml:math id="M1346" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:mi mathvariant="normal">C</mml:mi></mml:mrow></mml:math></inline-formula> uncertainty of <inline-formula><mml:math id="M1347" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1348" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">‰</mml:mi></mml:mrow></mml:math></inline-formula> required to differentiate between source types corresponds to a <inline-formula><mml:math id="M1349" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> uncertainty of <inline-formula><mml:math id="M1350" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.02</mml:mn></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M1351" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula>. Significant spatial and/or temporal averaging is therefore required to reduce uncertainties to detectable levels. In addition, <inline-formula><mml:math id="M1352" display="inline"><mml:mrow class="chem"><mml:msup><mml:mi/><mml:mn mathvariant="normal">13</mml:mn></mml:msup><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> retrievals are highly sensitive to errors in a priori temperature and pressure profiles, which can introduce systematic biases <xref ref-type="bibr" rid="bib1.bibx66" id="paren.305"/>. A dedicated detectability assessment will be essential to evaluate whether current or forthcoming missions can effectively detect and interpret atmospheric isotopic variations under real conditions.</p>
</sec>

      
      </body>
    <back><app-group>
        <supplementary-material position="anchor"><p id="d2e18879">The supplement related to this article is available online at <inline-supplementary-material xlink:href="https://doi.org/10.5194/essd-18-4793-2026-supplement" xlink:title="pdf">https://doi.org/10.5194/essd-18-4793-2026-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d2e18890">ET compiled and aggregated the isotopic datasets, performed temporal extrapolations, designed and carried out the simulation experiments, and analyzed the results. AB and MS contributed to the study design, supervised the project, and supported the interpretation of results and manuscript preparation. AM processed the meteorological mass fluxes used to drive the transport model, contributed data processing scripts, and provided technical support for implementation in the Community Inversion Framework. MN and XL provided source-specific isotopic datasets. MM, JT, DG, and EM provided expertise on isotopic datasets and feedback on the analysis. ET prepared the manuscript with contributions from all co-authors.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d2e18896">The contact author has declared that none of the authors has any competing interests.</p>
  </notes><notes notes-type="disclaimer"><title>Disclaimer</title>

      <p id="d2e18902">Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this paper. The authors bear the ultimate responsibility for providing appropriate place names. Views expressed in the text are those of the authors and do not necessarily reflect the views of the publisher.</p>
  </notes><ack><title>Acknowledgements</title><p id="d2e18908">This work was also  conducted in the frame of the ESA initiative SMART-CH4 (Satellite Monitoring of Atmospheric Methane), which is part of the EC-ESA Joint Earth System Science Initiative. This work was granted access to the HPC resources of TGCC under the allocations A0140102201 made by GENCI.</p><p id="d2e18910">Finally, we wish to thank J. Bruna (LSCE) and his team for computer support and the use of the OBELIX computing facility at LSCE.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d2e18915">This research has been supported by the European Space Agency (grant no. 4000142730/23/I-NS).</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d2e18921">This paper was edited by Yuqiang Zhang and reviewed by two anonymous referees.</p>
  </notes><ref-list>
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