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  <front>
    <journal-meta><journal-id journal-id-type="publisher">ACP</journal-id><journal-title-group>
    <journal-title>Atmospheric Chemistry and Physics</journal-title>
    <abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">Atmos. Chem. Phys.</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">1680-7324</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/acp-24-577-2024</article-id><title-group><article-title>Zonal variability of methane trends derived<?xmltex \hack{\break}?> from satellite data</article-title><alt-title>Zonal variability of methane trends derived from satellite data</alt-title>
      </title-group><?xmltex \runningtitle{Zonal variability of methane trends derived from satellite data}?><?xmltex \runningauthor{J. Hachmeister~et~al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes">
          <name><surname>Hachmeister</surname><given-names>Jonas</given-names></name>
          <email>jonas_h@iup.physik.uni-bremen.de</email>
        <ext-link>https://orcid.org/0000-0001-5700-4502</ext-link></contrib>
        <contrib contrib-type="author" corresp="no">
          <name><surname>Schneising</surname><given-names>Oliver</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-1725-8246</ext-link></contrib>
        <contrib contrib-type="author" corresp="no">
          <name><surname>Buchwitz</surname><given-names>Michael</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-7616-1837</ext-link></contrib>
        <contrib contrib-type="author" corresp="no">
          <name><surname>Burrows</surname><given-names>John P.</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-1547-8130</ext-link></contrib>
        <contrib contrib-type="author" corresp="no">
          <name><surname>Notholt</surname><given-names>Justus</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no">
          <name><surname>Buschmann</surname><given-names>Matthias</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-5077-9524</ext-link></contrib>
        <aff id="aff1"><institution>Institute of Environmental Physics (IUP), University of Bremen FB1, Bremen, Germany</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Jonas Hachmeister (jonas_h@iup.physik.uni-bremen.de)</corresp></author-notes><pub-date><day>15</day><month>January</month><year>2024</year></pub-date>
      
      <volume>24</volume>
      <issue>1</issue>
      <fpage>577</fpage><lpage>595</lpage>
      <history>
        <date date-type="received"><day>24</day><month>July</month><year>2023</year></date>
           <date date-type="accepted"><day>1</day><month>December</month><year>2023</year></date>
           <date date-type="rev-recd"><day>1</day><month>December</month><year>2023</year></date>
           <date date-type="rev-request"><day>11</day><month>August</month><year>2023</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2024 </copyright-statement>
        <copyright-year>2024</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://acp.copernicus.org/articles/.html">This article is available from https://acp.copernicus.org/articles/.html</self-uri><self-uri xlink:href="https://acp.copernicus.org/articles/.pdf">The full text article is available as a PDF file from https://acp.copernicus.org/articles/.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d1e125">The Tropospheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor (S5P) satellite is part of the latest generation of trace gas monitoring satellites and provides a new level of spatio-temporal information with daily global coverage, which enables the calculation of daily globally averaged <inline-formula><mml:math id="M1" display="inline"><mml:mrow class="chem"><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. To investigate changes in atmospheric methane, the background <inline-formula><mml:math id="M2" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> level (i.e. the <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> concentration without seasonal and short-term variations) has to be determined. <inline-formula><mml:math id="M4" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> growth rates vary in a complex manner and high-latitude zonal averages may have gaps in the time series, and thus simple fitting methods do not produce reliable results. In this paper we present an approach based on fitting an ensemble of dynamic linear models (DLMs) to TROPOMI data, from which the best model is chosen with the help of cross-validation to prevent overfitting. This method is computationally fast and is not dependent on additional inputs, allowing for fast and continuous analysis of the most recent time series data. We present results of global annual methane increases (AMIs) for the first 4.5 years of S5P/TROPOMI data, which show good agreement with AMIs from other sources. Additionally, we investigated what information can be derived from zonal bands. Due to the fast meridional mixing within hemispheres, we use zonal growth rates instead of AMIs, since they provide a higher temporal resolution. Clear differences can be observed between Northern Hemisphere and Southern Hemisphere growth rates, especially during 2019 and 2022. The growth rates show similar patterns within the hemispheres and show no short-term variations during the years, indicating that air masses within a hemisphere are well-mixed during a year. Additionally, the growth rates derived from S5P/TROPOMI data are largely consistent with growth rates derived from Copernicus Atmospheric Monitoring Service (CAMS) global-inversion-optimized (CAMS/INV) data, which use surface observations. In 2019 a reduction in growth rates can be observed for the Southern Hemisphere, while growth rates in the Northern Hemisphere stay stable or increase. During 2020 a strong increase in Southern Hemisphere growth rates can be observed, which is in accordance with recently reported increases in Southern Hemisphere wetland emissions. In 2022 the reduction in the global AMI can be attributed to decreased growth rates in the Northern Hemisphere, while growth rates in the Southern Hemisphere remain high. Investigations of fluxes from CAMS/INV data support these observations and suggest that the Northern Hemisphere decrease is mainly due to the decrease in anthropogenic fluxes, while in the Southern Hemisphere, wetland fluxes continued to rise. While the continued increase in Southern Hemisphere wetland fluxes agrees with existing studies about the causes of observed methane trends, the difference between Northern Hemisphere and Southern Hemisphere methane increases in 2022 has not been discussed before and calls for further research.</p>
  </abstract>
    
<funding-group>
<award-group id="gs1">
<funding-source>Universität Bremen</funding-source>
<award-id>n/a</award-id>
</award-group>
<award-group id="gs2">
<funding-source>Deutsche Forschungsgemeinschaft</funding-source>
<award-id>268020496</award-id>
<award-id>INST 144/379-1</award-id>
<award-id>INST 144/493-1</award-id>
</award-group>
<award-group id="gs3">
<funding-source>European Space Agency</funding-source>
<award-id>4000126450/19/I-NB</award-id>
<award-id>4000137895/22/I-AG</award-id>
</award-group>
<award-group id="gs4">
<funding-source>Bundesministerium für Bildung und Forschung</funding-source>
<award-id>01 LK2103A</award-id>
</award-group>
</funding-group>
</article-meta>
  </front>
<body>
      

      <?xmltex \bartext{Research article}?>
<?pagebreak page578?><sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e183">Methane (<inline-formula><mml:math id="M5" display="inline"><mml:mrow class="chem"><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 one of the most important drivers of climate change with an effective radiative forcing of 1.19 <inline-formula><mml:math id="M6" 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>
<xref ref-type="bibr" rid="bib1.bibx1" id="paren.1"/> and an atmospheric lifetime of 9.1 years <xref ref-type="bibr" rid="bib1.bibx49" id="paren.2"/>. The short lifespan of <inline-formula><mml:math id="M7" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> compared to other greenhouse gases and the large fraction of anthropogenic emissions make <inline-formula><mml:math id="M8" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emission reduction an attractive strategy to slow down or possibly reduce human-made climate change in the short to medium term. Accurate knowledge of the atmospheric <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> concentrations and dry column mixing ratios is therefore essential for improving our knowledge of the sources and sinks of <inline-formula><mml:math id="M10" display="inline"><mml:mrow class="chem"><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 science and international environmental policy. The globally averaged surface concentration of <inline-formula><mml:math id="M11" display="inline"><mml:mrow class="chem"><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 by 156 % between 1750 and 2019, reaching 1866 <inline-formula><mml:math id="M12" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 3.3 <inline-formula><mml:math id="M13" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> in 2019 <xref ref-type="bibr" rid="bib1.bibx22" id="paren.3"/> and 1917.11 <inline-formula><mml:math id="M14" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> in June 2023 <xref ref-type="bibr" rid="bib1.bibx33" id="paren.4"/>.</p>
      <p id="d1e306">While the concentrations have risen in total, the trend, i.e. the rate of change in the background level without seasonal or short-term variations, has evolved non-linearly. Global methane concentrations have been observed to increase in the period from the 1980s to 2000 and from 2007 to the present. However, a plateau between 2000 and 2007 was observed. This is referred to as “stabilization”. Whether to define the stabilization period or the period of renewed growth (2007–present) as anomalous has been a subject of debate. There have been a variety of explanations for the observed behaviour in the literature <xref ref-type="bibr" rid="bib1.bibx50" id="paren.5"/>. Recent publications suggest that the period of renewed growth can be attributed to the rise in microbial emissions <xref ref-type="bibr" rid="bib1.bibx32 bib1.bibx2" id="paren.6"/> and the fact that tropical methane emissions explain the majority of recent changes in the atmospheric methane growth rate <xref ref-type="bibr" rid="bib1.bibx18" id="paren.7"/>. In 2020 and 2021, record methane increases were observed by the Global Monitoring Laboratory of the National Oceanic and Atmospheric Administration (NOAA-GML) <xref ref-type="bibr" rid="bib1.bibx33" id="paren.8"/> and the Copernicus Climate Change Service (C3S) <xref ref-type="bibr" rid="bib1.bibx11" id="paren.9"/>. The reasons for these increases are still debated, with studies attributing them to increases in wetland emissions and changes in the atmospheric methane sink to varying degrees. The main sink of methane is through reaction with the hydroxyl radical (OH) in the troposphere. The rate of this reaction depends on the concentration of OH, which is determined by its photochemical sources and sinks. Recent studies suggest that the steep decline of nitrogen dioxide (<inline-formula><mml:math id="M15" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">NO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) <xref ref-type="bibr" rid="bib1.bibx6" id="paren.10"/>, carbon monoxide (CO), and non-methane volatile organic compound emissions as a result of the measures introduced to control and limit the spread of the COVID-19 pandemic lowered the levels of OH and thus led to part of the increase in <inline-formula><mml:math id="M16" display="inline"><mml:mrow class="chem"><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 in 2020 and 2021 <xref ref-type="bibr" rid="bib1.bibx48 bib1.bibx34 bib1.bibx38 bib1.bibx41 bib1.bibx19" id="paren.11"/>. Additionally, enhanced wetland emissions, especially from tropical wetlands, contributed to the record increases in atmospheric <inline-formula><mml:math id="M17" display="inline"><mml:mrow class="chem"><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 2020 and 2021 <xref ref-type="bibr" rid="bib1.bibx38 bib1.bibx19 bib1.bibx18 bib1.bibx41" id="paren.12"/>.</p>
      <p id="d1e367">The Arctic contains large amounts of soil organic carbon (SOC), which is stored in the permafrost regions (ca. 1300 <inline-formula><mml:math id="M18" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Pg</mml:mi></mml:mrow></mml:math></inline-formula>), of which roughly 800 <inline-formula><mml:math id="M19" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">Pg</mml:mi></mml:mrow></mml:math></inline-formula> is perennially frozen <xref ref-type="bibr" rid="bib1.bibx26" id="paren.13"/>. The comparatively high temperature increase in the Arctic, compared to the rest of the world and also called “Arctic amplification” <xref ref-type="bibr" rid="bib1.bibx45 bib1.bibx52" id="paren.14"/>, may lead to increased permafrost degradation and rapid SOC loss <xref ref-type="bibr" rid="bib1.bibx40" id="paren.15"/> by the release of carbon dioxide (<inline-formula><mml:math id="M20" 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>) and/or methane. Latitudinally resolved growth rates are especially interesting in this regard and provided the initial motivation for this study.</p>
      <p id="d1e407">In this paper we present methane growth rates and annual methane increases (AMIs) derived from Sentinel-5P TROPOMI <inline-formula><mml:math id="M21" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data using a dynamic linear model (DLM) approach. In the second section we present the data used. Next, we describe our method for calculating these growth rates, which is divided into four parts: (i) we discuss the preparation of the data; (ii) we provide a brief introduction to DLMs; (iii) we discuss our ensemble approach, which utilizes cross-validation to find the optimal DLM configuration for a given time series; and (iv) we provide a method to calculate a bias related to the satellite sampling. In the fourth section we present global AMIs for the first 4.5 years of Sentinel-5 Precursor (S5P) TROPOMI data and compare these to AMIs from other sources. In the fifth section we investigate zonal growth rates derived from 20<inline-formula><mml:math id="M22" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> latitudinal bands to provide spatial information to the global AMIs. Additionally, we compare the growth rates to growth rates derived from Copernicus Atmospheric Monitoring Service (CAMS) global inversion-optimized methane data (CAMS/INV) which assimilate either surface observations or surface and satellite data. In the sixth section we investigate CAMS/INV fluxes to help with the interpretation of our previous results. Finally, we summarize our results and discuss potential future uses of this method and suggestions for further research. In the Appendix we provide additional information about our method and further results which are not included in the main text.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Data</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Sentinel-5P TROPOMI WFMD product</title>
      <?pagebreak page579?><p id="d1e445">The S5P satellite was launched on 13 October 2017 and has since delivered high-quality data from its only scientific instrument, TROPOMI, which is a nadir-viewing passive grating imaging spectrometer. Combined with a near-polar, sun-synchronous orbit, the swath width of 2600 <inline-formula><mml:math id="M23" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:math></inline-formula> provides daily global coverage. Due to the orbit geometry and swath overlap, multiple observations per day are possible in the polar regions. The spatial resolution depends on the bands and is 5.5 <inline-formula><mml:math id="M24" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 7 <inline-formula><mml:math id="M25" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">km</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> for the short-wave infrared (SWIR) band (7 <inline-formula><mml:math id="M26" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 7 <inline-formula><mml:math id="M27" display="inline"><mml:mrow class="unit"><mml:msup><mml:mi mathvariant="normal">km</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:math></inline-formula> before August 2019) <xref ref-type="bibr" rid="bib1.bibx35" id="paren.16"/>. Methane is retrieved from TROPOMI measurements of sunlight reflected by the Earth's surface and atmosphere in the SWIR wavelengths. We use the latest release of the Weighting Function Modified Differential Optical Absorption Spectroscopy (WFMD) product (v1.8) <xref ref-type="bibr" rid="bib1.bibx43" id="paren.17"/>, which includes processing improvements such as an increased polynomial degree (cubic instead of quadratic) and an updated digital elevation model to account for various localized topography-related biases <xref ref-type="bibr" rid="bib1.bibx24" id="paren.18"/>. Furthermore, the machine-learning-based quality filter in the post-processing is improved to further reduce scenes with residual clouds. We use data with a quality flag <inline-formula><mml:math id="M28" display="inline"><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">qf</mml:mi></mml:mrow><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:math></inline-formula> (good) and do not include data with <inline-formula><mml:math id="M29" display="inline"><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">qf</mml:mi></mml:mrow><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> (potentially bad). The WFMD product includes measurements for solar zenith angles up to 75<inline-formula><mml:math id="M30" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>. We performed this analysis using data from May 2018 to February 2023, excluding data from the commissioning phase (November 2017 to April 2018). Uncertainties for these data are estimated during the inversion procedure via error propagation from the spectral measurement errors given in the TROPOMI Level-1 files. Additionally, the uncertainties include a correction by statistically comparing the original uncertainties to the measured scatter relative to Total Carbon Column Observing Network (TCCON) measurements.</p>
</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>CAMS global inversion-optimized greenhouse gas fluxes and concentrations (CAMS/INV)</title>
      <p id="d1e545">The CAMS/INV dataset provides data for carbon dioxide, nitrous oxide, and methane. The methane data are produced using the CAMS <inline-formula><mml:math id="M31" display="inline"><mml:mrow class="chem"><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 inversion system <xref ref-type="bibr" rid="bib1.bibx44" id="paren.19"/>, which is based on the TM5-4DVar inverse modelling system <xref ref-type="bibr" rid="bib1.bibx3 bib1.bibx4" id="paren.20"/>. We use release v22r1, where only ground-based observations from the NOAA network are used in the inversion (CAMS/INV-SRF), and release v21r1s, which includes satellite observations from the Greenhouse Gases Observing Satellite (GOSAT) in addition to ground-based observations (CAMS/INV-SRF-SAT). In our analysis we use the total column dry-air mole fractions and surface fluxes of methane from this dataset. The data are provided on a 2<inline-formula><mml:math id="M32" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M33" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 3<inline-formula><mml:math id="M34" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> grid from 1990 to 2022. We only apply our DLM approach to the methane concentrations from these data and use the corresponding fluxes directly to help with interpretation.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <label>2.3</label><?xmltex \opttitle{NOAA {$\protect\chem{CH_{{4}}}$} marine boundary layer reference}?><title>NOAA <inline-formula><mml:math id="M35" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> marine boundary layer reference</title>
      <p id="d1e611">The marine boundary layer reference (MBLR) is a two-dimensional matrix (time vs. latitude) created from weekly air samples from the Cooperative Air Sampling Network <xref ref-type="bibr" rid="bib1.bibx16" id="paren.21"/>, which is created for various long-lived trace gases by NOAA–GML. The MBLR is created by first fitting the weekly data whereby the <inline-formula><mml:math id="M36" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> level, seasonal component, and short-term variations are separated. For each time step (48 evenly distributed per year) the different stations give a latitudinal distribution of <inline-formula><mml:math id="M37" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> which is then smoothed. The global mean is calculated by averaging the smoothed latitudinal distribution for each time step. A detailed explanation can be found on the NOAA website <xref ref-type="bibr" rid="bib1.bibx37" id="paren.22"/>.</p>
</sec>
<sec id="Ch1.S2.SS4">
  <label>2.4</label><title>University of Bremen C3S/CAMS satellite data (UB–C3S–CAMS)</title>
      <p id="d1e650">Annual methane increases are published by the Copernicus Climate Change Service (C3S, <xref ref-type="bibr" rid="bib1.bibx9" id="altparen.23"/>) in the context of the European State of the Climate (ESOTC) assessment. Here we use data from the ESOTC 2022 <xref ref-type="bibr" rid="bib1.bibx12" id="paren.24"/> climate indicator section <xref ref-type="bibr" rid="bib1.bibx11" id="paren.25"/>. The methane data as shown on that website are (i) time series of monthly values of the column-averaged mole fraction of atmospheric methane, <inline-formula><mml:math id="M38" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, as derived from satellite data; and (ii) annual mean methane growth rates including uncertainty estimates as derived from this time series.</p>
      <p id="d1e673">The <inline-formula><mml:math id="M39" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> time series corresponds to averaged satellite data over land in the latitude band 60<inline-formula><mml:math id="M40" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S–60<inline-formula><mml:math id="M41" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N and covers the period January 2003 to December 2022. The underlying satellite <inline-formula><mml:math id="M42" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data product for 2002–2021 is XCH4_OBS4MIPS version 4.4 available from the Copernicus Climate Data Store (CDS,<xref ref-type="bibr" rid="bib1.bibx10" id="altparen.26"/>) website <xref ref-type="bibr" rid="bib1.bibx8" id="paren.27"/>. The data product is derived from the satellite instruments SCIAMACHY/ENVISAT, TANSO-FTS/GOSAT, and TANSO-FTS-2/GOSAT-2. A previous version of this data product is described in <xref ref-type="bibr" rid="bib1.bibx42" id="text.28"/>. This dataset is extended using a year 2022 satellite-derived <inline-formula><mml:math id="M43" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data product generated for CAMS <xref ref-type="bibr" rid="bib1.bibx7" id="paren.29"/> (see <xref ref-type="bibr" rid="bib1.bibx11" id="altparen.30"/>, for details).</p>
      <p id="d1e743">The combined C3S/CAMS <inline-formula><mml:math id="M44" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> time series has been generated by the University of Bremen (UB) and is in the following referred to as the UB–C3S–CAMS dataset. This dataset is also used to derive annual mean methane growth rates for 2003–2022 using the method as described in <xref ref-type="bibr" rid="bib1.bibx5" id="text.31"/> for <inline-formula><mml:math id="M45" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>, which was later also applied to <inline-formula><mml:math id="M46" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> <xref ref-type="bibr" rid="bib1.bibx42" id="paren.32"/>. This method provides a new time series from the monthly <inline-formula><mml:math id="M47" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> time series described above. The new time series is generated by computing the difference in <inline-formula><mml:math id="M48" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> for a given calendar month between 2 consecutive years (e.g. January 2019 and 2020). The time assigned to this difference is the mean time between the 2 months (e.g. mid-July 2019). The annual mean growth rate for a given year is the weighted average of all monthly difference values of that year.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><?xmltex \currentcnt{1}?><?xmltex \def\figurename{Figure}?><label>Figure 1</label><caption><p id="d1e811"><bold>(a)</bold> Temporal inhomogeneity (<inline-formula><mml:math id="M49" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) for global <inline-formula><mml:math id="M50" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> WFMDv1.8 data between May 2018 and February 2023. Grid cells with <inline-formula><mml:math id="M51" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M52" display="inline"><mml:mo>&gt;</mml:mo></mml:math></inline-formula> 0.5 are omitted during analysis. <bold>(b)</bold> Spatial inhomogeneity (<inline-formula><mml:math id="M53" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) for global <inline-formula><mml:math id="M54" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> WFMDv1.8 data. Days above the <inline-formula><mml:math id="M55" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> threshold (black line) are omitted from analysis, and the threshold is set by Eq. (<xref ref-type="disp-formula" rid="Ch1.E5"/>), which was empirically chosen.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f01.png"/>

        </fig>

</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Method</title>
      <p id="d1e910">The Method section is split into four parts. First, we describe how the data are prepared for the DLM, meaning how we get from single observations to a time series we can fit our model to. Next, we briefly introduce DLMs and provide information on the specific types of models we are using. In<?pagebreak page580?> the third subsection we explain how we use an ensemble of DLMs and cross-validation to select the best model. Lastly, we describe how we estimate the bias related to imperfect satellite sampling.</p>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Data preparation</title>
      <p id="d1e920">The <inline-formula><mml:math id="M56" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data to be used in the DLM fitting are pre-processed onto a latitude–longitude grid with sufficiently homogeneous sampling in space and time. Initially, the WFMD <inline-formula><mml:math id="M57" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data product is gridded onto a 2<inline-formula><mml:math id="M58" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M59" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 2<inline-formula><mml:math id="M60" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> grid. For this we assign each measurement to a single grid cell and calculate the weighted average of all measurements per cell. The measurements are weighted using the inverse measurement uncertainty to disadvantage measurements with high uncertainty. For example, reported uncertainties are higher for low-albedo scenes. Thus, these scenes contribute less to the average. The coverage of the WFMD data is roughly 25 % in all regions and is mostly constant, except for a few days with lower coverage and the seasonal data gaps at high latitudes (see Fig. <xref ref-type="fig" rid="App1.Ch1.S4.F18"/>). To account for inhomogeneities in spatial and temporal sampling, we apply the method described by <xref ref-type="bibr" rid="bib1.bibx46" id="text.33"/>. This method quantifies the sampling distribution's inhomogeneity using a measure denoted as <inline-formula><mml:math id="M61" display="inline"><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>≤</mml:mo><mml:mi>H</mml:mi><mml:mo>≤</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>, which is defined as a linear combination of the asymmetry <inline-formula><mml:math id="M62" display="inline"><mml:mi>A</mml:mi></mml:math></inline-formula> and entropy <inline-formula><mml:math id="M63" display="inline"><mml:mi>E</mml:mi></mml:math></inline-formula> of the data.

                <disp-formula specific-use="align" content-type="numbered"><mml:math id="M64" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="Ch1.E1"><mml:mtd><mml:mtext>1</mml:mtext></mml:mtd><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mi>H</mml:mi><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mn mathvariant="normal">2</mml:mn></mml:mfrac></mml:mstyle><mml:mo>(</mml:mo><mml:mi>A</mml:mi><mml:mo>+</mml:mo><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>-</mml:mo><mml:mi>E</mml:mi><mml:mo>)</mml:mo><mml:mo>)</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E2"><mml:mtd><mml:mtext>2</mml:mtext></mml:mtd><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mi>A</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi mathvariant="normal">|</mml:mi><mml:mover accent="true"><mml:mi>x</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover><mml:mo>-</mml:mo><mml:msub><mml:mi>x</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub><mml:mi mathvariant="normal">|</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi>x</mml:mi></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E3"><mml:mtd><mml:mtext>3</mml:mtext></mml:mtd><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mi>E</mml:mi><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mrow><mml:msub><mml:mtext>log</mml:mtext><mml:mi mathvariant="normal">e</mml:mi></mml:msub><mml:mo>(</mml:mo><mml:mi>N</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:mfrac></mml:mstyle><mml:munder><mml:mo movablelimits="false">∑</mml:mo><mml:mi>i</mml:mi></mml:munder><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi>n</mml:mi><mml:mo>(</mml:mo><mml:mi>i</mml:mi><mml:mo>)</mml:mo></mml:mrow><mml:mrow><mml:msub><mml:mi>n</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfrac></mml:mstyle><mml:msub><mml:mtext>log</mml:mtext><mml:mi mathvariant="normal">e</mml:mi></mml:msub><mml:mfenced close=")" open="("><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mi>n</mml:mi><mml:mo>(</mml:mo><mml:mi>i</mml:mi><mml:mo>)</mml:mo></mml:mrow><mml:mrow><mml:msub><mml:mi>n</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:mfrac></mml:mstyle></mml:mfenced></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula></p>
      <p id="d1e1165">In Eq. (<xref ref-type="disp-formula" rid="Ch1.E2"/>), the mean location of measurements is given by <inline-formula><mml:math id="M65" display="inline"><mml:mover accent="true"><mml:mi>x</mml:mi><mml:mo mathvariant="normal">‾</mml:mo></mml:mover></mml:math></inline-formula> (e.g. mean spatial position or mean time), <inline-formula><mml:math id="M66" display="inline"><mml:mrow><mml:msub><mml:mi>x</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> is the central point, and <inline-formula><mml:math id="M67" display="inline"><mml:mrow><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi>x</mml:mi></mml:mrow></mml:math></inline-formula> is the width of the region. Equation (<xref ref-type="disp-formula" rid="Ch1.E3"/>) represents the normalized entropy with <inline-formula><mml:math id="M68" display="inline"><mml:mi>N</mml:mi></mml:math></inline-formula> as the number of bins (e.g. grid cells or time steps), <inline-formula><mml:math id="M69" display="inline"><mml:mrow><mml:mi>n</mml:mi><mml:mo>(</mml:mo><mml:mi>i</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> the number of observations in bin <inline-formula><mml:math id="M70" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula>, and <inline-formula><mml:math id="M71" display="inline"><mml:mrow><mml:msub><mml:mi>n</mml:mi><mml:mn mathvariant="normal">0</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> the sample size.</p>
      <p id="d1e1243"><inline-formula><mml:math id="M72" display="inline"><mml:mi>A</mml:mi></mml:math></inline-formula> can be intuitively understood as the asymmetry of the sampling distribution. For example, <inline-formula><mml:math id="M73" display="inline"><mml:mi>A</mml:mi></mml:math></inline-formula> would be high if only measurements in the Eastern Hemisphere are present for a given day. In contrast, <inline-formula><mml:math id="M74" display="inline"><mml:mi>A</mml:mi></mml:math></inline-formula> would be zero if the measurements are symmetrically distributed around the central point. The normalized entropy is <inline-formula><mml:math id="M75" display="inline"><mml:mrow><mml:mi>E</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> for perfectly homogeneous sampling patterns and decreases for each missing measurement. The entropy does however not capture the distribution of the sampling pattern. Hence, a combination of both measures is used to quantify the homogeneity of the sampling distribution. Values of <inline-formula><mml:math id="M76" display="inline"><mml:mi>H</mml:mi></mml:math></inline-formula> close to zero indicate a homogeneous sampling distribution, while values close to one indicate a very inhomogeneous distribution. Inaccurate estimates and spurious features can arise without accounting for this inhomogeneous sampling <xref ref-type="bibr" rid="bib1.bibx46" id="paren.34"/>. The inhomogeneity can be calculated in the temporal domain (for each grid cell) and in the spatial domain (for each time step).</p>
      <p id="d1e1288">We first calculate the temporal inhomogeneity (<inline-formula><mml:math id="M77" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) for each grid cell, which quantifies how evenly and symmetrically the data for each grid cell are distributed in the temporal domain. <inline-formula><mml:math id="M78" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> tends to be higher in cells with sparse data coverage, which are often found over the oceans and tropical rainforests due to high cloud coverage (see Fig. <xref ref-type="fig" rid="Ch1.F1"/>). We then filter cells with <inline-formula><mml:math id="M79" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msub><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn></mml:mrow></mml:math></inline-formula>. This threshold value was chosen empirically to exclude cells in these regions with limited cloud-free coverage. Next, we calculate the spatial inhomogeneity (<inline-formula><mml:math id="M80" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) within the designated sub-grid, such as a zonal band. This allows us to identify days with very inhomogeneous coverage. The spatial inhomogeneity can be calculated along both spatial dimensions. Hence, we define <inline-formula><mml:math id="M81" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> as the equally weighted linear combination of the latitudinal and longitudinal spatial inhomogeneity:
            <disp-formula id="Ch1.E4" content-type="numbered"><label>4</label><mml:math id="M82" display="block"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn><mml:mo>⋅</mml:mo><mml:msubsup><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi><mml:mtext>lat</mml:mtext></mml:msubsup><mml:mo>+</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn><mml:mo>⋅</mml:mo><mml:msubsup><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi><mml:mtext>lon</mml:mtext></mml:msubsup><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p id="d1e1392">We determine a limit, <inline-formula><mml:math id="M83" display="inline"><mml:mrow><mml:msubsup><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi><mml:mtext>lim</mml:mtext></mml:msubsup></mml:mrow></mml:math></inline-formula>, as the median of <inline-formula><mml:math id="M84" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> plus 2 standard deviations,
            <disp-formula id="Ch1.E5" content-type="numbered"><label>5</label><mml:math id="M85" display="block"><mml:mrow><mml:msubsup><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi><mml:mtext>lim</mml:mtext></mml:msubsup><mml:mo>=</mml:mo><mml:msub><mml:mover accent="true"><mml:mi>H</mml:mi><mml:mo stretchy="false" mathvariant="normal">̃</mml:mo></mml:mover><mml:mi mathvariant="normal">S</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi></mml:msub></mml:mrow></mml:msub><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
          and filter out days with <inline-formula><mml:math id="M86" display="inline"><mml:mrow><mml:msub><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi></mml:msub><mml:mo>&gt;</mml:mo><mml:msubsup><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi><mml:mtext>lim</mml:mtext></mml:msubsup></mml:mrow></mml:math></inline-formula>. The equation for <inline-formula><mml:math id="M87" display="inline"><mml:mrow><mml:msubsup><mml:mi>H</mml:mi><mml:mi mathvariant="normal">S</mml:mi><mml:mtext>lim</mml:mtext></mml:msubsup></mml:mrow></mml:math></inline-formula> was empirically chosen and yields reliable limits for different sub-grids. Figure <xref ref-type="fig" rid="Ch1.F1"/> illustrates the spatial and temporal inhomogeneity for global WFMDv1.8 data.</p>
      <p id="d1e1493">Finally, we compute the area-weighted average of the chosen sub-grid, generating a time series for the analysis. To further mitigate sampling bias in the global average, we first average over longitudes and subsequently over latitudes. This approach assumes a faster mixing of background methane levels within zonal bands while acknowledging greater latitudinal disparities. A more detailed description is given in Sect. <xref ref-type="sec" rid="Ch1.S3.SS4"/>. CAMS/INV <inline-formula><mml:math id="M88" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data are already provided on a grid with complete coverage, and no inhomogeneity treatment is necessary. The time series are therefore calculated<?pagebreak page581?> using the area-weighted average of the sub-grid. Since the DLM approach is based on the assumption that errors are present and normally distributed, we add a Gaussian noise with <inline-formula><mml:math id="M89" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> <inline-formula><mml:math id="M90" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> 0.2 <inline-formula><mml:math id="M91" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> to the CAMS/INV <inline-formula><mml:math id="M92" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> time series.</p>
</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><title>Dynamic linear model fit</title>
      <p id="d1e1551">To extract information about the methane growth rate from the time series we first need to calculate the underlying <inline-formula><mml:math id="M93" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> level, that is the smoothly changing background concentration without seasonal or short-term variation. While a simple approach, such as fitting a polynomial plus a trigonometric function to model the seasonality, may be considered, it is insufficient due to the complex change in <inline-formula><mml:math id="M94" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> levels observed in historical records <xref ref-type="bibr" rid="bib1.bibx33 bib1.bibx11" id="paren.35"/>. The use of a moving average is not suitable due to possible data gaps, especially for high-latitude bands. Therefore, we employ dynamic linear models to fit the <inline-formula><mml:math id="M95" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data, which allow for the trend (i.e. the slope of the level, the growth rate) to change over time and can deal with missing data. For the analysis of global methane growth we use AMIs, similar to other relevant studies <xref ref-type="bibr" rid="bib1.bibx15 bib1.bibx11 bib1.bibx43" id="paren.36"/>. This enables the methane growth of different studies to be readily compared. AMIs are defined as the difference in methane level between 1 January of 2 consecutive years. This is a measure of the integrated growth rate over the same time span. For zonal bands we directly investigate the growth rate instead of AMIs (see Sect. <xref ref-type="sec" rid="Ch1.S5"/> for a more detailed description).</p>
      <p id="d1e1596">A dynamic linear model is a regression model that can handle observations of varying accuracy, missing data, non-uniform sampling, and non-stationary processes. It allows some of its parameters to change over time and directly models the observed variability using unobserved state variables <xref ref-type="bibr" rid="bib1.bibx30" id="paren.37"/>. These DLM properties allow the analysis of not only global but also zonal methane data, which can have higher uncertainties and more gaps, especially at higher latitudes. Additionally, the direct modelling of the data allows partitioning of the signal into different components, such as an underlying level and seasonal component, which can prove advantageous beyond the scope of this paper.</p>
      <p id="d1e1602">A DLM can be formulated as a special case of a state-space model, i.e. a model which consists of some unobserved components (represented by a state vector) and the observation vector. The evolution of the state vector and the relation between observation and state vectors are modelled by a set of equations. If these equations are linear, we have a so-called dynamic linear model. The DLM we use consists of three main components: first, a slowly changing background level, which captures the long-term trend of the methane concentration; second, a seasonal component included to model variations arising from seasonal cycles. This component enables variations in the phase and amplitude of the seasonal cycle to be accounted for. Third, an autoregressive component is incorporated to model noise and residual correlations in the data, accounting for short-term effects. Additionally, Gaussian noise can be included to model part of the errors. The ability of DLMs to capture changing components over time is achieved by modelling these changes as Gaussian random walks, allowing for smooth transitions and adjustments. The variances of these Gaussian random walks determine the overall variability of a certain parameter (e.g. trend). A detailed description of the model set-up and the different DLM components can be found in Appendix <xref ref-type="sec" rid="App1.Ch1.S1"/>.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><?xmltex \currentcnt{2}?><?xmltex \def\figurename{Figure}?><label>Figure 2</label><caption><p id="d1e1610">DLM fit for daily area-weighted global WFMDv1.8 data. Panel <bold>(a)</bold> shows the daily area-weighted global <inline-formula><mml:math id="M96" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> together with the level and level + seasonal components from the DLM fit. <bold>(b)</bold> The trend or growth rate is the slope of the level, the dashed lines show the 1<inline-formula><mml:math id="M97" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> uncertainty, panel <bold>(c)</bold> shows the seasonal component which captures the seasonal cycle, panel <bold>(d)</bold> shows the AR(1) component capturing residual correlations in the data, <bold>(e)</bold> the residual shows the difference between the fit and the data, and <bold>(f)</bold> a histogram of the residual shows that it is roughly normally distributed.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f02.png"/>

        </fig>

      <p id="d1e1656">In general, the model parameters (e.g. variances; see Table <xref ref-type="table" rid="App1.Ch1.S1.T4"/> for a complete list) are not known beforehand and have to be determined. For this purpose, maximum likelihood estimation (MLE) <xref ref-type="bibr" rid="bib1.bibx17 bib1.bibx25" id="paren.38"/> can be used. MLE is a statistical method that estimates the parameters of a model by maximizing the likelihood of the observed data given the model's assumptions. Note that the data uncertainties are not used in the MLE but are indirectly included during the data preparation (gridding) as described above. For the end-user, various software packages exist which provide the implementation of this procedure, leaving only the model configuration open for the user. In our study we use the UnobservedComponents class of the statsmodel Python package (version 0.14.0, <xref ref-type="bibr" rid="bib1.bibx39" id="altparen.39"/>), which provides the means to define a DLM and to fit it using MLE (see <xref ref-type="bibr" rid="bib1.bibx47" id="text.40"/> for documentation). An overview of a DLM fit for globally averaged WFMD data can be seen in Fig. <xref ref-type="fig" rid="Ch1.F2"/>.</p>
      <?pagebreak page582?><p id="d1e1672">DLMs have been previously used to successfully model stratospheric ozone <xref ref-type="bibr" rid="bib1.bibx31" id="paren.41"/>, methane from different GOSAT retrievals to investigate the seasonal cycle and trend <xref ref-type="bibr" rid="bib1.bibx29" id="paren.42"/>, and methane from ground-based remote sensing <xref ref-type="bibr" rid="bib1.bibx28" id="paren.43"/>. For a detailed description of DLMs, including their formulation as a special case of a state-space model, we refer readers to <xref ref-type="bibr" rid="bib1.bibx17" id="text.44"/> and <xref ref-type="bibr" rid="bib1.bibx25" id="text.45"/>. For a more concise introduction to DLMs, we refer readers to <xref ref-type="bibr" rid="bib1.bibx30" id="text.46"/>.</p>
</sec>
<sec id="Ch1.S3.SS3">
  <label>3.3</label><title>Ensemble approach and cross-validation</title>
      <p id="d1e1702">The choice of model configuration is a non-trivial problem, which is impacted by prior knowledge, empirical testing, and different quality measures. From prior knowledge the inclusion of a seasonal component is inferred, because the existence of a seasonality in atmospheric methane concentrations is known. Empirical testing can show that the inclusion of an autoregressive component is necessary, because the data contain residual short-term variations. The term “quality measures” refers to measures that facilitate model selection, such as the mean squared error (MSE), which is defined as the mean of squared differences between the model and data. Additionally, the DLM provides variances (squared standard deviations) for each component which can be used to compare models; models with lower uncertainty in the level and seasonality are preferable to models with high uncertainties for these terms.</p>
      <p id="d1e1705">To avoid the need for manual model selection, we employ an ensemble approach, fitting a range of DLMs to the data and automatically selecting the best model. The ensemble consists of different DLM configurations, with varying components as described in Appendix <xref ref-type="sec" rid="App1.Ch1.S1"/>. Additionally, we perform <inline-formula><mml:math id="M98" display="inline"><mml:mi>k</mml:mi></mml:math></inline-formula>-fold cross-validation (CV) with <inline-formula><mml:math id="M99" display="inline"><mml:mrow><mml:mi>k</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> folds for each DLM to calculate an average mean squared error (AMSE). During CV, the DLM is fitted on a portion of the data while leaving out another portion (the fold) for testing. The difference between the model fit and the fold is used to calculate the MSE, and the average MSE across all five folds per DLM provides the AMSE. Low AMSE values indicate a better model fit and help in selecting the best model for a given time series. The final model selection is based on an aggregated score, defined as the sum of the AMSE, the variance of the level, and the variance of the seasonal term:
            <disp-formula id="Ch1.E6" content-type="numbered"><label>6</label><mml:math id="M100" display="block"><mml:mrow><mml:msub><mml:mi>S</mml:mi><mml:mtext>agg</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">AMSE</mml:mi></mml:mrow><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>level</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>seas</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p id="d1e1764">The inclusion of the variances ensures that the uncertainty of the level and seasonal components is considered in the selection criterion. This approach aims to select DLMs that provide good estimates of the underlying methane signal while avoiding overfitting and reliance on expert knowledge.</p>
      <p id="d1e1767">Different methods and measures can be used for model selection and may yield different results. We want to emphasize that the problem of model selection is non-trivial, and different approaches may be suitable for different data and use cases. Here we select the model which yields the highest certainty fit of the level and seasonal component (i.e. the <inline-formula><mml:math id="M101" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> signal without noise) while avoiding overfitting and manual selection. Furthermore, we want to mention that, in most cases, the differences between all the models in an ensemble are rather small, with the best models producing approximately the same results. However, the use of a single DLM configuration for all zonal bands is not feasible due to the inherent differences in the seasonal signal for each zonal band. Additionally, an over-specified model can lead to high uncertainties in the resulting fit.</p>
      <p id="d1e1782">To quantify the impact of model selection, we calculate a model selection bias <inline-formula><mml:math id="M102" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>model</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:math></inline-formula>, which is included in the error budget of all the AMIs and growth rates. For global data we calculate the AMIs for all the models in an ensemble and determine the weighted variance for each year of interest:
            <disp-formula id="Ch1.E7" content-type="numbered"><label>7</label><mml:math id="M103" display="block"><mml:mtable class="split" rowspacing="0.2ex" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mtext>Model</mml:mtext><mml:mo>/</mml:mo><mml:mtext>AMI,j</mml:mtext></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>=</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mspace linebreak="nobreak" width="0.25em"/><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mo>∑</mml:mo><mml:mi>i</mml:mi></mml:msub><mml:mo>(</mml:mo><mml:msub><mml:mrow class="chem"><mml:mi mathvariant="normal">AMI</mml:mi></mml:mrow><mml:mrow><mml:mtext>avg</mml:mtext><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mrow class="chem"><mml:mi mathvariant="normal">AMI</mml:mi></mml:mrow><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:msubsup><mml:mover accent="true"><mml:mi mathvariant="italic">σ</mml:mi><mml:mo mathvariant="normal" stretchy="false">̃</mml:mo></mml:mover><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msubsup></mml:mrow><mml:mrow><mml:msub><mml:mo>∑</mml:mo><mml:mi>i</mml:mi></mml:msub><mml:msup><mml:msub><mml:mover accent="true"><mml:mi mathvariant="italic">σ</mml:mi><mml:mo mathvariant="normal" stretchy="false">̃</mml:mo></mml:mover><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:mfrac></mml:mstyle><mml:mo>;</mml:mo></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mspace linebreak="nobreak" width="0.25em"/><mml:msubsup><mml:mover accent="true"><mml:mi mathvariant="italic">σ</mml:mi><mml:mo stretchy="false" mathvariant="normal">̃</mml:mo></mml:mover><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>=</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mtext>avg</mml:mtext><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula>
          where <inline-formula><mml:math id="M104" display="inline"><mml:mrow><mml:msub><mml:mrow class="chem"><mml:mi mathvariant="normal">AMI</mml:mi></mml:mrow><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the AMI for year <inline-formula><mml:math id="M105" display="inline"><mml:mi>j</mml:mi></mml:math></inline-formula> and model <inline-formula><mml:math id="M106" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M107" display="inline"><mml:mrow><mml:msub><mml:mrow class="chem"><mml:mi mathvariant="normal">AMI</mml:mi></mml:mrow><mml:mrow><mml:mtext>avg</mml:mtext><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> the average AMI of all models in year <inline-formula><mml:math id="M108" display="inline"><mml:mi>j</mml:mi></mml:math></inline-formula>, and <inline-formula><mml:math id="M109" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mtext>avg</mml:mtext><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M110" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> the corresponding uncertainties as given by the DLM. For the case of growth rates we calculate a single model uncertainty which is averaged over all time steps:
            <disp-formula id="Ch1.E8" content-type="numbered"><label>8</label><mml:math id="M111" display="block"><mml:mtable class="split" rowspacing="0.2ex" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mtext>Model</mml:mtext><mml:mo>/</mml:mo><mml:mtext>trend</mml:mtext></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>=</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mspace width="0.25em" linebreak="nobreak"/><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mn mathvariant="normal">1</mml:mn><mml:mi>T</mml:mi></mml:mfrac></mml:mstyle><mml:munder><mml:mo movablelimits="false">∑</mml:mo><mml:mi>t</mml:mi></mml:munder><mml:mfenced open="[" close="]"><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:msub><mml:mo>∑</mml:mo><mml:mi>i</mml:mi></mml:msub><mml:mo>(</mml:mo><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mrow><mml:mtext>avg</mml:mtext><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:msup><mml:msub><mml:mover accent="true"><mml:mi mathvariant="italic">σ</mml:mi><mml:mo mathvariant="normal" stretchy="false">̃</mml:mo></mml:mover><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow><mml:mrow><mml:msub><mml:mo>∑</mml:mo><mml:mi>i</mml:mi></mml:msub><mml:msup><mml:msub><mml:mover accent="true"><mml:mi mathvariant="italic">σ</mml:mi><mml:mo stretchy="false" mathvariant="normal">̃</mml:mo></mml:mover><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:mfrac></mml:mstyle></mml:mfenced><mml:mo>;</mml:mo></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mspace linebreak="nobreak" width="0.25em"/><mml:msup><mml:msub><mml:mover accent="true"><mml:mi mathvariant="italic">σ</mml:mi><mml:mo mathvariant="normal" stretchy="false">̃</mml:mo></mml:mover><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>=</mml:mo><mml:msup><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mtext>avg</mml:mtext><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>+</mml:mo><mml:msup><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula>
          where <inline-formula><mml:math id="M112" display="inline"><mml:mi>T</mml:mi></mml:math></inline-formula> is the total number of time steps, <inline-formula><mml:math id="M113" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> the growth rate for model <inline-formula><mml:math id="M114" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> at time step <inline-formula><mml:math id="M115" display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M116" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mrow><mml:mtext>avg</mml:mtext><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> the average growth rate of all models at time step <inline-formula><mml:math id="M117" display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M118" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mtext>avg</mml:mtext><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> the uncertainty of the average growth rate at time step <inline-formula><mml:math id="M119" display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula>, and <inline-formula><mml:math id="M120" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>t</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> the uncertainty of model <inline-formula><mml:math id="M121" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> at time step <inline-formula><mml:math id="M122" display="inline"><mml:mi>t</mml:mi></mml:math></inline-formula> as given by the DLM.</p>
      <p id="d1e2335">The contribution of the model selection bias to the error budget can be seen in Table <xref ref-type="table" rid="Ch1.T1"/> for global AMIs and in Table <xref ref-type="table" rid="Ch1.T2"/> for zonal growth rates. In the case of global data, the contribution is small for all years with <inline-formula><mml:math id="M123" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Model</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> <inline-formula><mml:math id="M124" display="inline"><mml:mo>&lt;</mml:mo></mml:math></inline-formula> 1 <inline-formula><mml:math id="M125" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> except for 2018, when only an incomplete time series is available. For zonal data, <inline-formula><mml:math id="M126" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Model</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> varies between the bands and is in the range of 1.03–4.34 <inline-formula><mml:math id="M127" 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>.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1"><?xmltex \currentcnt{1}?><label>Table 1</label><caption><p id="d1e2400">Error budget for global AMIs. <inline-formula><mml:math id="M128" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>DLM</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is the uncertainty provided by the DLM fit, <inline-formula><mml:math id="M129" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Model</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is the uncertainty from model selection, and <inline-formula><mml:math id="M130" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Sampling</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is the bias due to satellite sampling. All values show 1<inline-formula><mml:math id="M131" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> uncertainties.</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="right"/>
     <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 rowsep="1">
         <oasis:entry colname="col1">Year</oasis:entry>
         <oasis:entry colname="col2">2018<inline-formula><mml:math id="M133" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">2019</oasis:entry>
         <oasis:entry colname="col4">2020</oasis:entry>
         <oasis:entry colname="col5">2021</oasis:entry>
         <oasis:entry colname="col6">2022</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M134" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>DLM</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">1.70</oasis:entry>
         <oasis:entry colname="col3">0.40</oasis:entry>
         <oasis:entry colname="col4">0.39</oasis:entry>
         <oasis:entry colname="col5">0.39</oasis:entry>
         <oasis:entry colname="col6">0.49</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M135" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Model</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">3.22</oasis:entry>
         <oasis:entry colname="col3">0.71</oasis:entry>
         <oasis:entry colname="col4">0.32</oasis:entry>
         <oasis:entry colname="col5">0.48</oasis:entry>
         <oasis:entry colname="col6">0.35</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M136" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Sampling</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">2.96</oasis:entry>
         <oasis:entry colname="col3">0.25</oasis:entry>
         <oasis:entry colname="col4">0.19</oasis:entry>
         <oasis:entry colname="col5">0.26</oasis:entry>
         <oasis:entry colname="col6">0.25</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M137" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mtext>Sampling</mml:mtext><mml:mo>(</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">SZA</mml:mi></mml:mrow><mml:mo>)</mml:mo></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">0.06</oasis:entry>
         <oasis:entry colname="col3">0.37</oasis:entry>
         <oasis:entry colname="col4">0.05</oasis:entry>
         <oasis:entry colname="col5">0.22</oasis:entry>
         <oasis:entry colname="col6">0.73</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M138" 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></oasis:entry>
         <oasis:entry colname="col2">4.70</oasis:entry>
         <oasis:entry colname="col3">0.85</oasis:entry>
         <oasis:entry colname="col4">0.53</oasis:entry>
         <oasis:entry colname="col5">0.67</oasis:entry>
         <oasis:entry colname="col6">0.65</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><table-wrap-foot><p id="d1e2443">All values are in parts per billion. <inline-formula><mml:math id="M132" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula> 2018 only includes data starting on 1 May 2018.</p></table-wrap-foot><?xmltex \gdef\@currentlabel{1}?></table-wrap>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T2"><?xmltex \currentcnt{2}?><label>Table 2</label><caption><p id="d1e2675">Sampling and model error for zonal growth rates. <inline-formula><mml:math id="M139" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>DLM</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> is not included in this table since it varies with time but is shown in Fig. <xref ref-type="fig" rid="Ch1.F8"/>. All values show 1<inline-formula><mml:math id="M140" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> uncertainties.</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="right"/>
     <oasis:colspec colnum="4" colname="col4" align="right"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Band</oasis:entry>
         <oasis:entry colname="col2"><inline-formula><mml:math id="M141" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Model</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M142" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Sampling</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col4"><inline-formula><mml:math id="M143" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mtext>Sampling</mml:mtext><mml:mo>(</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">SZA</mml:mi></mml:mrow><mml:mo>)</mml:mo></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">70–90<inline-formula><mml:math id="M144" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col2">1.44</oasis:entry>
         <oasis:entry colname="col3">2.70</oasis:entry>
         <oasis:entry colname="col4">0.14</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">50–70<inline-formula><mml:math id="M145" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col2">1.92</oasis:entry>
         <oasis:entry colname="col3">1.30</oasis:entry>
         <oasis:entry colname="col4">0.61</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">30–50<inline-formula><mml:math id="M146" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col2">1.87</oasis:entry>
         <oasis:entry colname="col3">1.46</oasis:entry>
         <oasis:entry colname="col4">0.00</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">10–30<inline-formula><mml:math id="M147" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col2">3.63</oasis:entry>
         <oasis:entry colname="col3">1.52</oasis:entry>
         <oasis:entry colname="col4">0.00</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M148" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>10–10<inline-formula><mml:math id="M149" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N</oasis:entry>
         <oasis:entry colname="col2">3.34</oasis:entry>
         <oasis:entry colname="col3">2.65</oasis:entry>
         <oasis:entry colname="col4">0.00</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">10–30<inline-formula><mml:math id="M150" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S</oasis:entry>
         <oasis:entry colname="col2">1.73</oasis:entry>
         <oasis:entry colname="col3">1.87</oasis:entry>
         <oasis:entry colname="col4">0.00</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">30–50<inline-formula><mml:math id="M151" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S</oasis:entry>
         <oasis:entry colname="col2">1.03</oasis:entry>
         <oasis:entry colname="col3">3.98</oasis:entry>
         <oasis:entry colname="col4">0.00</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">50–70<inline-formula><mml:math id="M152" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S</oasis:entry>
         <oasis:entry colname="col2">2.95</oasis:entry>
         <oasis:entry colname="col3">1.46</oasis:entry>
         <oasis:entry colname="col4">1.85</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">70–90<inline-formula><mml:math id="M153" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S</oasis:entry>
         <oasis:entry colname="col2">4.34</oasis:entry>
         <oasis:entry colname="col3">1.94</oasis:entry>
         <oasis:entry colname="col4">0.67</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><table-wrap-foot><p id="d1e2698">All values are given in parts per billion per year.</p></table-wrap-foot><?xmltex \gdef\@currentlabel{2}?></table-wrap>

</sec>
<sec id="Ch1.S3.SS4">
  <label>3.4</label><title>Estimation of sampling bias</title>
      <?pagebreak page583?><p id="d1e3003">The spatio-temporal coverage of S5P <inline-formula><mml:math id="M154" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data is limited mostly by cloud coverage, the polar nights, and poorly reflective surfaces, while additional gaps may exist due to technical problems with the satellite platform. Additionally, the sampling distribution is not completely random but is influenced by the total land mass per latitudinal band and seasonal cloud coverage over the tropical and subtropical oceans. The daily gridded data for S5P <inline-formula><mml:math id="M155" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> are therefore always incomplete, meaning we have some grid cells without any measurements. Here we investigate the systematic sampling bias due to polar nights, the total effect due to sampling, and the effect of the averaging method. For this, we use CAMS/INV <inline-formula><mml:math id="M156" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data (see Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>), onto which we apply different masks and averaging methods. Since CAMS/INV data have a complete coverage (due to being model data), we can investigate the effects of different sampling masks or averaging and compare them to the results gained from the unmasked data.</p>
      <p id="d1e3041">We therefore compare AMIs (for global data) and growth rates (for zonal data) calculated using different samplings and/or methods. To simulate the spatio-temporal pattern of S5P sampling, we created a daily mask from gridded WFMDv1.8 data and applied it to the model data. To only simulate the systematic effect of the polar nights, we created a daily mask using the average solar zenith angle (SZA) per grid cell with a cut-off value of 75<inline-formula><mml:math id="M157" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>. The AMIs and growth rates for CAMS/INV <inline-formula><mml:math id="M158" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data were calculated using the same ensemble approach used for WFMD data.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e3066">Global AMIs derived from CAMS/INV-SRF <inline-formula><mml:math id="M159" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data using <bold>(a)</bold> the non-masked dataset with standard averaging, <bold>(b)</bold> the S5P-sampled CAMS/INV-SRF data with standard averaging, and <bold>(c)</bold> the S5P-sampled CAMS/INV-SRF data using our zonal-first averaging approach.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f03.png"/>

        </fig>

      <p id="d1e3096">First, we investigate the effect of the averaging method. We compare standard averaging, which is defined in this study as the area-weighted mean of all grid cells in a region, with an approach we call zonal-first averaging. Zonal-first averaging takes into account the inhomogeneous sampling at each latitude, which is influenced by the distribution of land mass and seasonal coverage. Since zonal transport occurs within weeks <xref ref-type="bibr" rid="bib1.bibx27" id="paren.47"/>, we first average the grid cells zonally, assuming that the available data within a 2<inline-formula><mml:math id="M160" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> band provide a good estimate of the mean <inline-formula><mml:math id="M161" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> at this latitude. For global data this means that we first average the data in all 90 2<inline-formula><mml:math id="M162" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> latitude bands, and for zonal growth rates this would mean first averaging the 10 2<inline-formula><mml:math id="M163" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> latitude bands within a 20<inline-formula><mml:math id="M164" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> zonal band. Subsequently, we calculate the average from the zonal averages, which leads to a consistent weighting of all the latitudes regardless of their individual coverage. Figure <xref ref-type="fig" rid="Ch1.F3"/> shows AMIs calculated from CAMS/INV-SRF <inline-formula><mml:math id="M165" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data using (a) no mask and standard averaging, (b) the S5P <inline-formula><mml:math id="M166" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mask and standard averaging, and (c) the S5P <inline-formula><mml:math id="M167" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mask and zonal-first averaging. Using zonal-first averaging, the AMIs are closer to the AMIs derived from the complete data. This is especially visible for 2020, where the AMI is overestimated by roughly 3 <inline-formula><mml:math id="M168" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> when using the standard averaging. Therefore, we use zonal-first averaging for all calculations of globally averaged data.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e3195">Zonal growth rates derived from CAMS/INV-SRF <inline-formula><mml:math id="M169" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data using <bold>(a)</bold> the non-masked dataset with zonal-first averaging, <bold>(b)</bold> the S5P-sampled CAMS/INV-SRF data with standard averaging, and <bold>(c)</bold> the S5P-sampled CAMS/INV-SRF data using our zonal-first averaging approach.</p></caption>
          <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f04.png"/>

        </fig>

      <p id="d1e3224">Figure <xref ref-type="fig" rid="Ch1.F4"/> shows zonal growth rates calculated from CAMS/INV-SRF <inline-formula><mml:math id="M170" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data using (a) no mask and standard averaging, (b) the S5P <inline-formula><mml:math id="M171" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mask and standard averaging, and (c) the S5P <inline-formula><mml:math id="M172" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mask and zonal-first averaging. Growth rates calculated on the masked data show 1<inline-formula><mml:math id="M173" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> agreement with the growth rates calculated on the complete data. Growth rates calculated using the zonal-first averaging show better agreement for the 50–70<inline-formula><mml:math id="M174" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>S band, while for the 10<inline-formula><mml:math id="M175" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>S–10<inline-formula><mml:math id="M176" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>N band the growth rate is more variable. For all the other zonal bands the results are nearly identical. Noticeably, the 70–90<inline-formula><mml:math id="M177" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula>N band shows no variation when using the S5P <inline-formula><mml:math id="M178" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mask, indicating that insufficient data coverage hinders the detection of growth rate variation. Since sampling within a 20<inline-formula><mml:math id="M179" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> zonal band can still vary with latitude, we follow the same reasoning as in the previous paragraph and also use zonal-first averaging for zonal growth rate calculation.</p>
      <?pagebreak page584?><p id="d1e3326">The different growth rates for Fig. <xref ref-type="fig" rid="Ch1.F4"/>a–c indicate the presence of a sampling bias. Thus, we investigated the effect of satellite sampling and the polar nights by applying corresponding masks to CAMS/INV <inline-formula><mml:math id="M180" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data. For global data the sampling biases are calculated by taking the squared difference between the AMIs calculated on the complete data (without any sampling filtering) and the AMIs calculated on the masked CAMS/INV data. We calculate a separate bias for each year in our analysis.

                <disp-formula specific-use="align" content-type="numbered"><mml:math id="M181" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="Ch1.E9"><mml:mtd><mml:mtext>9</mml:mtext></mml:mtd><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Sampling</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>=</mml:mo><mml:mo>(</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">AMI</mml:mi></mml:mrow><mml:mo>-</mml:mo><mml:msub><mml:mrow class="chem"><mml:mi mathvariant="normal">AMI</mml:mi></mml:mrow><mml:mtext>Sampling</mml:mtext></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="Ch1.E10"><mml:mtd><mml:mtext>10</mml:mtext></mml:mtd><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>SZA</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>=</mml:mo><mml:mo>(</mml:mo><mml:mrow class="chem"><mml:mi mathvariant="normal">AMI</mml:mi></mml:mrow><mml:mo>-</mml:mo><mml:msub><mml:mrow class="chem"><mml:mi mathvariant="normal">AMI</mml:mi></mml:mrow><mml:mtext>SZA</mml:mtext></mml:msub><mml:msup><mml:mo>)</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula></p>
      <p id="d1e3419">Table <xref ref-type="table" rid="Ch1.T1"/> shows the resulting errors for global AMIs. The sampling bias is around 0.25 <inline-formula><mml:math id="M182" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> for all fully available years and is much higher for 2018 with 2.96 <inline-formula><mml:math id="M183" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula>. The contribution of the SZA-related bias varies from year to year with a maximum value of 0.73 <inline-formula><mml:math id="M184" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> in the year 2022. This variability might be related to the varying difference between the high and mid latitudes during the different years. When the difference between both is bigger, the masking of high-latitude regions is expected to have a larger effect on AMIs.  For the analysis of zonal bands we calculate a zonal error by taking the average squared difference between growth rates derived from the complete data and growth rates derived from the reduced CAMS/INV <inline-formula><mml:math id="M185" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data for each band:
            <disp-formula id="Ch1.E11" content-type="numbered"><label>11</label><mml:math id="M186" display="block"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mtext>Sampling</mml:mtext><mml:mo>/</mml:mo><mml:mtext>Zonal</mml:mtext></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>=</mml:mo><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:mi>i</mml:mi><mml:mi>N</mml:mi></mml:munderover><mml:msup><mml:mfenced open="(" close=")"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mi>i</mml:mi></mml:msub><mml:mo>-</mml:mo><mml:msubsup><mml:mi mathvariant="italic">ν</mml:mi><mml:mi>i</mml:mi><mml:mtext>Sampling</mml:mtext></mml:msubsup></mml:mrow></mml:mfenced><mml:mn mathvariant="normal">2</mml:mn></mml:msup><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
          where <inline-formula><mml:math id="M187" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mi>i</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the growth rate at time step <inline-formula><mml:math id="M188" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M189" display="inline"><mml:mi>N</mml:mi></mml:math></inline-formula> is the total number of data points. The sampling errors for zonal growth rates are shown in Table <xref ref-type="table" rid="Ch1.T2"/>. Higher sampling errors correlate clearly with regions of high temporal inhomogeneity, which further shows the challenging sampling conditions in these regions (see Fig. <xref ref-type="fig" rid="Ch1.F1"/>).</p>
</sec>
</sec>
<sec id="Ch1.S4">
  <label>4</label><title>Comparison of different global annual methane increases</title>
      <p id="d1e3553">In this section, we discuss the global AMIs calculated using WFMDv1.8 data from May 2018 to February 2023. The results are shown in Fig. <xref ref-type="fig" rid="Ch1.F5"/>. An overall, although non-linear, rise in the methane level is observed between 2019 and 2022. The most significant change occurs from 2019 to 2020, with an increase from 6.89 <inline-formula><mml:math id="M190" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.85 <inline-formula><mml:math id="M191" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> to 14.40 <inline-formula><mml:math id="M192" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.53 <inline-formula><mml:math id="M193" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula>. The highest AMI is observed in 2021, reaching 16.93 <inline-formula><mml:math id="M194" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.67 <inline-formula><mml:math id="M195" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula>. The globally averaged <inline-formula><mml:math id="M196" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> rose from 1817.32 <inline-formula><mml:math id="M197" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 2.81 <inline-formula><mml:math id="M198" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> at the beginning of 2018 to 1878.14 <inline-formula><mml:math id="M199" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.16 <inline-formula><mml:math id="M200" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">ppb</mml:mi></mml:mrow></mml:math></inline-formula> at the end of 2022.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><?xmltex \currentcnt{5}?><?xmltex \def\figurename{Figure}?><label>Figure 5</label><caption><p id="d1e3648">Global annual methane increases derived from Sentinel-5P TROPOMI WFMDv1.8 data. The error bars show the 1<inline-formula><mml:math id="M201" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> uncertainty and include the DLM, sampling, and model error.</p></caption>
        <?xmltex \igopts{width=207.705118pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f05.png"/>

      </fig>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T3" specific-use="star"><?xmltex \currentcnt{3}?><label>Table 3</label><caption><p id="d1e3667">Comparison of global AMIs using different data and methods.</p></caption><oasis:table frame="topbot"><?xmltex \begin{scaleboxenv}{.96}[.96]?><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="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:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Method@Dataset (time resolution)</oasis:entry>
         <oasis:entry colname="col2">2018</oasis:entry>
         <oasis:entry colname="col3">2019</oasis:entry>
         <oasis:entry colname="col4">2020</oasis:entry>
         <oasis:entry colname="col5">2021</oasis:entry>
         <oasis:entry colname="col6">2022</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">DLM@WFMDv1.8 (daily)</oasis:entry>
         <oasis:entry colname="col2">9.74 <inline-formula><mml:math id="M204" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4.70<inline-formula><mml:math id="M205" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">6.89 <inline-formula><mml:math id="M206" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.85</oasis:entry>
         <oasis:entry colname="col4">14.40 <inline-formula><mml:math id="M207" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.53</oasis:entry>
         <oasis:entry colname="col5">16.93 <inline-formula><mml:math id="M208" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.67</oasis:entry>
         <oasis:entry colname="col6">12.72 <inline-formula><mml:math id="M209" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.65</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">DLM@WFMDv1.8 (monthly)</oasis:entry>
         <oasis:entry colname="col2">6.56 <inline-formula><mml:math id="M210" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 4.23<inline-formula><mml:math id="M211" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3">7.85 <inline-formula><mml:math id="M212" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.98</oasis:entry>
         <oasis:entry colname="col4">14.39 <inline-formula><mml:math id="M213" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.93</oasis:entry>
         <oasis:entry colname="col5">16.55 <inline-formula><mml:math id="M214" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.94</oasis:entry>
         <oasis:entry colname="col6">12.65 <inline-formula><mml:math id="M215" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.17</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><xref ref-type="bibr" rid="bib1.bibx43" id="text.48"/> @WFMDv1.8 (monthly)</oasis:entry>
         <oasis:entry colname="col2"/>
         <oasis:entry colname="col3">7.80 <inline-formula><mml:math id="M216" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.60</oasis:entry>
         <oasis:entry colname="col4">15.00 <inline-formula><mml:math id="M217" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.00</oasis:entry>
         <oasis:entry colname="col5">16.40 <inline-formula><mml:math id="M218" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.50</oasis:entry>
         <oasis:entry colname="col6">13.90 <inline-formula><mml:math id="M219" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.60</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">NOAA–GML (version 2023-10) @NOAA MBLR (daily)<inline-formula><mml:math id="M220" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">8.76 <inline-formula><mml:math id="M221" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.52</oasis:entry>
         <oasis:entry colname="col3">9.68 <inline-formula><mml:math id="M222" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.60</oasis:entry>
         <oasis:entry colname="col4">15.16 <inline-formula><mml:math id="M223" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.41</oasis:entry>
         <oasis:entry colname="col5">17.82 <inline-formula><mml:math id="M224" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.47</oasis:entry>
         <oasis:entry colname="col6">13.97 <inline-formula><mml:math id="M225" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.58</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">DLM@NOAA MBLR (daily)<inline-formula><mml:math id="M226" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">9.35 <inline-formula><mml:math id="M227" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.89</oasis:entry>
         <oasis:entry colname="col3">8.60 <inline-formula><mml:math id="M228" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.75</oasis:entry>
         <oasis:entry colname="col4">15.99 <inline-formula><mml:math id="M229" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.97</oasis:entry>
         <oasis:entry colname="col5">18.16 <inline-formula><mml:math id="M230" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.22</oasis:entry>
         <oasis:entry colname="col6">16.04 <inline-formula><mml:math id="M231" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.86</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><xref ref-type="bibr" rid="bib1.bibx5" id="text.49"/> @UB–C3S–CAMS (monthly)</oasis:entry>
         <oasis:entry colname="col2">10.19 <inline-formula><mml:math id="M232" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.96</oasis:entry>
         <oasis:entry colname="col3">9.00 <inline-formula><mml:math id="M233" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 2.01</oasis:entry>
         <oasis:entry colname="col4">15.19 <inline-formula><mml:math id="M234" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 2.09</oasis:entry>
         <oasis:entry colname="col5">17.09 <inline-formula><mml:math id="M235" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 2.09</oasis:entry>
         <oasis:entry colname="col6">11.87 <inline-formula><mml:math id="M236" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 2.77</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">DLM@UB–C3S–CAMS (monthly)</oasis:entry>
         <oasis:entry colname="col2">10.15 <inline-formula><mml:math id="M237" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.13</oasis:entry>
         <oasis:entry colname="col3">8.92 <inline-formula><mml:math id="M238" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.30</oasis:entry>
         <oasis:entry colname="col4">15.77 <inline-formula><mml:math id="M239" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.20</oasis:entry>
         <oasis:entry colname="col5">17.04 <inline-formula><mml:math id="M240" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.05</oasis:entry>
         <oasis:entry colname="col6">11.46 <inline-formula><mml:math id="M241" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 1.96</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">DLM@CAMS/INV–SURF (daily)</oasis:entry>
         <oasis:entry colname="col2">6.24 <inline-formula><mml:math id="M242" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.97</oasis:entry>
         <oasis:entry colname="col3">9.86 <inline-formula><mml:math id="M243" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.39</oasis:entry>
         <oasis:entry colname="col4">13.34 <inline-formula><mml:math id="M244" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.38</oasis:entry>
         <oasis:entry colname="col5">18.04 <inline-formula><mml:math id="M245" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.71</oasis:entry>
         <oasis:entry colname="col6">15.33 <inline-formula><mml:math id="M246" display="inline"><mml:mo>±</mml:mo></mml:math></inline-formula> 0.48</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup><?xmltex \end{scaleboxenv}?></oasis:table><?xmltex \begin{scaleboxenv}{.96}[.96]?><table-wrap-foot><p id="d1e3670"><?xmltex \hack{\vspace*{2mm}}?>All values are in parts per billion. Uncertainties reflect 1 standard deviation. <inline-formula><mml:math id="M202" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula> Larger error since only data starting with May 2018 were used. <inline-formula><mml:math id="M203" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula> Input data have a weekly time resolution, but AMIs are provided as for daily data (as the difference between 1 January of 2 consecutive years).</p></table-wrap-foot><?xmltex \end{scaleboxenv}?><?xmltex \gdef\@currentlabel{3}?></table-wrap>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6"><?xmltex \currentcnt{6}?><?xmltex \def\figurename{Figure}?><label>Figure 6</label><caption><p id="d1e4226">Global annual methane increases derived from CAMS global inversion-optimized greenhouse gas concentrations including only surface observations. The error bars show the 1<inline-formula><mml:math id="M247" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> uncertainty and include the DLM and model error, which are also shown in brackets.</p></caption>
        <?xmltex \igopts{width=207.705118pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f06.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F7"><?xmltex \currentcnt{7}?><?xmltex \def\figurename{Figure}?><label>Figure 7</label><caption><p id="d1e4244">Comparison of global AMIs listed in Table <xref ref-type="table" rid="Ch1.T3"/>. The labels are formatted as Method@Dataset. Colours indicate the type of dataset used, and the markers denote the method. All errors represent 1<inline-formula><mml:math id="M248" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> uncertainties.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f07.png"/>

      </fig>

      <p id="d1e4262">To validate our findings, we compared our results with AMIs determined by <xref ref-type="bibr" rid="bib1.bibx43" id="text.50"/>, the NOAA–GML <xref ref-type="bibr" rid="bib1.bibx15" id="paren.51"/>, and data generated for the C3S <xref ref-type="bibr" rid="bib1.bibx11" id="paren.52"/>. Additionally, we include AMIs derived using our DLM approach for monthly WFMDv1.8 data, NOAA–GML MBLR data, and the UB–C3S–CAMS dataset. Table <xref ref-type="table" rid="Ch1.T3"/> and Fig. <xref ref-type="fig" rid="Ch1.F7"/> provide a comparison of AMIs between 2018 and 2022. While absolute values may differ due to variations in data and methods, all the AMIs exhibit the same qualitative trend. Differences are expected for various reasons. First, there is the difference in sampling. NOAA–GML AMIs are based on surface flask measurements rather than satellite total column observations used in the other calculations. Second, different methods are used to derive AMIs from the data (see the corresponding sources for descriptions of the other methods). Lastly, depending on the time<?pagebreak page585?> resolution of the data and the method used, the AMIs represent either the difference between 1 January of 2 consecutive years or the difference between the monthly January average of 2 consecutive years. The former is the case for our DLM approach and the AMIs derived by the NOAA–GML. The latter is the case for the AMIs derived by <xref ref-type="bibr" rid="bib1.bibx43" id="text.53"/> and for the C3S AMIs. To discern the impact of data and methodology, AMIs for the UB–C3S–CAMS and NOAA–GML datasets created using different methods can be compared. Our DLM-based AMIs of these datasets agree within 1<inline-formula><mml:math id="M249" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> with the calculations done for the C3S and by the NOAA–GML, indicating no significant differences due to the method used. However, we see a comparatively high AMI in 2022 for the combination of DLM and NOAA–GML data (see Fig. <xref ref-type="fig" rid="Ch1.F7"/>). This is probably related to the higher uncertainty for DLMs at the start and end of a time series, which can also be seen for UB–C3S-CAMS AMIs. A longer input time series will likely lead to a reduction in uncertainty and to a reduced deviation compared to the other 2022 AMIs. An application of our DLM approach for the complete UB–C3S–CAMS and NOAA–GML MBLR data can be seen in Appendix <xref ref-type="sec" rid="App1.Ch1.S2"/>.</p>
      <p id="d1e4293">Additionally, we used our DLM approach on monthly WFMDv1.8 data to better compare our method to the method used by <xref ref-type="bibr" rid="bib1.bibx43" id="text.54"/>, which also shows agreement within 1<inline-formula><mml:math id="M250" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>. Only differences smaller than 1<inline-formula><mml:math id="M251" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> are found when comparing AMIs based on the same data but different methods. We also applied our approach to CAMS/INV <inline-formula><mml:math id="M252" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data (see Sect. <xref ref-type="sec" rid="Ch1.S2.SS2"/>), for which global AMIs can be seen in Fig. <xref ref-type="fig" rid="Ch1.F6"/>. The AMIs are in qualitative agreement and show the same structure over the 5-year period; however, significant differences in absolute values are observed for 2020 and 2022. For 2020 the CAMS/INV AMI is significantly lower compared to most other sources, while for 2022 the CAMS/INV AMI is significantly higher compared to most other sources (see Table <xref ref-type="table" rid="Ch1.T3"/>).</p>
      <p id="d1e4331">The AMIs for 2020 and 2021 are the largest observed since the NOAA began systematic records in 1983. The drivers contributing to these record increases have been the subject<?pagebreak page586?> of recent debate and can be attributed to a rise in emissions, a reduction in the <inline-formula><mml:math id="M253" display="inline"><mml:mrow class="chem"><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, or a combination of both effects. According to the International Energy Agency (IEA), methane emissions from the energy sector decreased by approximately 10 % in 2020 <xref ref-type="bibr" rid="bib1.bibx20" id="paren.55"/>. However, additional emissions due to reduced maintenance of landfills and oil and gas infrastructure can be expected according to <xref ref-type="bibr" rid="bib1.bibx34" id="text.56"/>, while <xref ref-type="bibr" rid="bib1.bibx36" id="text.57"/> suggest that the effect of the global slowdown on anthropogenic <inline-formula><mml:math id="M254" display="inline"><mml:mrow class="chem"><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 is relatively small. Some studies propose that the reduction in the OH sink, caused by decreased emissions of nitrogen oxides during the COVID-19 pandemic, may explain part of the increase <xref ref-type="bibr" rid="bib1.bibx48 bib1.bibx34 bib1.bibx38 bib1.bibx41 bib1.bibx19" id="paren.58"/>. Specifically, <xref ref-type="bibr" rid="bib1.bibx48" id="text.59"/> and <xref ref-type="bibr" rid="bib1.bibx38" id="text.60"/> suggest that approximately half of the increase can be attributed to this effect. Conversely, several other studies attribute the majority of the <inline-formula><mml:math id="M255" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> increase in 2020 to the growth in wetland emissions <xref ref-type="bibr" rid="bib1.bibx41 bib1.bibx19 bib1.bibx18 bib1.bibx53" id="paren.61"/>.</p>
</sec>
<sec id="Ch1.S5">
  <label>5</label><title>Investigation of zonal methane growth rates</title>
      <p id="d1e4397">In addition to our global analysis, we investigated 20<inline-formula><mml:math id="M256" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> zonal bands. The good spatio-temporal coverage of S5P <inline-formula><mml:math id="M257" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> might suggest that the same approach of using AMIs could be applied to identify zonal bands with anomalous methane increases. However, the impact of atmospheric transport has to be considered. While longitudinal mixing occurs on timescales of a few weeks, meridional transport is slower, taking 1–2 months between mid-latitudes and the tropics or polar regions and around a year between hemispheres <xref ref-type="bibr" rid="bib1.bibx27 bib1.bibx51" id="paren.62"/>. The relatively longer atmospheric lifetime of 9.1 years <xref ref-type="bibr" rid="bib1.bibx49" id="paren.63"/> compared to the mixing times therefore guarantees a relatively even latitudinal distribution of methane in the troposphere, where the main difference is driven by the uneven distribution of <inline-formula><mml:math id="M258" display="inline"><mml:mrow class="chem"><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 <xref ref-type="bibr" rid="bib1.bibx51" id="paren.64"/>. Thus, we need to sample at about 1 year or less to observe differences between hemispheres and 1 month or less to observe differences within a hemisphere. The daily sampling of S5P is hence faster than meridional transport; however, part of the temporal information gets lost when using AMIs which are obtained by integrating the growth rate over 1 year. Thus, we investigate the growth rate, which is the trend component of our DLM fits, to obtain a better temporal resolution of the zonal signals.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F8"><?xmltex \currentcnt{8}?><?xmltex \def\figurename{Figure}?><label>Figure 8</label><caption><p id="d1e4443">Zonal growth rates for 20<inline-formula><mml:math id="M259" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> bands derived from <bold>(a)</bold> Sentinel-5P TROPOMI WFMDv1.8 data and <bold>(b)</bold> CAMS/INV-SRF <inline-formula><mml:math id="M260" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data. The errors show the 1<inline-formula><mml:math id="M261" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> uncertainty.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f08.png"/>

      </fig>

      <p id="d1e4485">The results are shown in Fig. <xref ref-type="fig" rid="Ch1.F8"/> and include growth rates derived from CAMS/INV-SRF <inline-formula><mml:math id="M262" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data for comparison. The shown errors include the uncertainty gained from the DLM fit <inline-formula><mml:math id="M263" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>DLM</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, the model selection error <inline-formula><mml:math id="M264" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Model</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula>, and the sampling error <inline-formula><mml:math id="M265" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>Sampling</mml:mtext></mml:msub></mml:mrow></mml:math></inline-formula> (see Sects. <xref ref-type="sec" rid="Ch1.S3.SS3"/> and <xref ref-type="sec" rid="Ch1.S3.SS4"/>). Growth rates are similar within a hemisphere, while differences between the hemispheres are clearly visible. Additionally, no significant sub-annual variations (i.e. on a monthly timescale) in zonal growth rates are present. Both observations are in good agreement with the known atmospheric mixing times and indicate that our data currently allow for identification of inter-hemispheric differences, while short-term variations between zonal bands are not detected. The high-latitude band between 70 and 90<inline-formula><mml:math id="M266" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N is included for completeness but shows no inter-annual variability. This may be due to a lack of real change in growth rates in this region, high uncertainties present in the data, and/or the sparse data coverage. The corresponding CAMS/INV-SRF <inline-formula><mml:math id="M267" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> growth rate indicates that the variability in the growth rate is relatively small in this band, which supports the first point of our explanation. We therefore exclude this band from our following discussion. Hence, we mean bands between 10 and 90<inline-formula><mml:math id="M268" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S when we speak of the Southern Hemisphere (SH) and bands between 10 and 70<inline-formula><mml:math id="M269" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N when we speak of the Northern Hemisphere (NH). The band between 10<inline-formula><mml:math id="M270" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S and 10<inline-formula><mml:math id="M271" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N represents the boundary region and is close to the global background, as can be seen in Fig. <xref ref-type="fig" rid="Ch1.F9"/>, which presents zonal growth rate anomalies. Zonal growth rate anomalies are defined as the difference between the zonal and global growth rates for each band.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F9"><?xmltex \currentcnt{9}?><?xmltex \def\figurename{Figure}?><label>Figure 9</label><caption><p id="d1e4601">Zonal growth rate anomalies for the 20<inline-formula><mml:math id="M272" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> bands derived from Sentinel-5P TROPOMI WFMDv1.8 data. The anomalies are defined as the differences between zonal and global growth rates.</p></caption>
        <?xmltex \igopts{width=179.252362pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f09.png"/>

      </fig>

      <?pagebreak page587?><p id="d1e4619">Overall growth rates derived from WFMD data are close to growth rates derived from CAMS/INV-SRF <inline-formula><mml:math id="M273" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data, with an overall agreement within 1<inline-formula><mml:math id="M274" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>. The growth rates and the growth rate anomalies can be used to interpret the changes in global AMIs and to allow the identification of hemispheres or zonal bands with anomalous growth rates. Differences between the hemispheres can be especially well seen in the zonal growth rate anomalies. During 2019 a decrease in growth rates can be observed for the whole SH (except for the southernmost band), while growth rates in the NH increased or stayed stable. For 2020 growth rates for all the SH bands increase greatly from roughly 0 to 20 <inline-formula><mml:math id="M275" 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>. The NH growth rates increase more slowly, except for the 50–70<inline-formula><mml:math id="M276" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N band, which exhibits a small decrease in the growth rate. During 2021 most zonal growth rates move towards or around the global mean, with the strongest anomaly visible in the 10–30<inline-formula><mml:math id="M277" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N band, which shows some additional increase in the growth rate that peaks in the middle of the year. During 2022 a clear difference between the hemispheres can be seen again, with a decrease in growth rates in the NH and an increase in or stabilization of growth rates in the SH. This difference is especially clear when looking at the zonal growth rate anomalies in Fig. <xref ref-type="fig" rid="Ch1.F9"/>.</p>
      <p id="d1e4678">Recent studies, which discuss the record methane increases in 2020 and 2021, can help with interpreting the structures of zonal growth rates. <xref ref-type="bibr" rid="bib1.bibx38" id="text.65"/> employ an atmospheric inversion using ground-based data. They attribute the increase from 2019 to 2020 roughly equally to changes in the OH sink and an increase in wetland emissions located mainly in the NH. In contrast, studies based on the inversion of satellite data from the Japanese Greenhouse gases Observing SATellite (GOSAT) state that the majority of increase from 2019 to 2020 can be attributed to the African continent <xref ref-type="bibr" rid="bib1.bibx19 bib1.bibx41" id="paren.66"/> with additional increases in tropical South America in 2021 <xref ref-type="bibr" rid="bib1.bibx19" id="paren.67"/>. Our findings can thus be seen as aligning with recent studies by <xref ref-type="bibr" rid="bib1.bibx19" id="text.68"/> and <xref ref-type="bibr" rid="bib1.bibx41" id="text.69"/>. The increase in SH growth rates from 2019 to 2020 is consistent with increased wetland emissions. The rise in the NH latitudinal bands during 2020 can be explained by the decreasing OH sink primarily located in the NH <xref ref-type="bibr" rid="bib1.bibx38 bib1.bibx19" id="paren.70"/>. However, the continued increase in 2021 cannot be solely explained by the OH sink, as OH levels mostly recovered in that year according to <xref ref-type="bibr" rid="bib1.bibx19" id="text.71"/> and <xref ref-type="bibr" rid="bib1.bibx38" id="text.72"/>. Possible explanations for the ongoing increase are persistent wetland emissions <xref ref-type="bibr" rid="bib1.bibx19" id="text.73"/> as well as the return to pre-pandemic methane emissions form the energy sector in 2021 <xref ref-type="bibr" rid="bib1.bibx21" id="paren.74"/>.  Finally, the decrease in growth rates in the NH and the increase in growth rates in the SH during 2022 have not been discussed to our knowledge. Our results therefore indicate that the decrease in global AMI from 2021 to 2022 can be attributed to a reduced growth rate in the NH. We investigate this further in the next section.</p>
</sec>
<sec id="Ch1.S6">
  <label>6</label><title>CAMS/INV fluxes</title>
      <p id="d1e4720">As mentioned before, zonal growth rates provide information about the change in methane concentration in a given zonal band, including changes in sources, sinks and transport patterns. These transport patterns would average out for global AMIs given a perfect coverage. In Sect. <xref ref-type="sec" rid="Ch1.S3.SS4"/> we applied a S5P <inline-formula><mml:math id="M278" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mask to CAMS/INV <inline-formula><mml:math id="M279" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data (see Fig. <xref ref-type="fig" rid="Ch1.F3"/>) and compared AMIs calculated from this masked data with AMIs calculated from the complete data. Since differences between these AMIs are small, we conclude that the effect of related sampling biases is limited. Therefore, changes in global AMIs can be attributed to the total source–sink balance of methane and not to changes in transport patterns. Whether this is also true for zonal growth rates is less clear, since transport effects are expected to be stronger especially within hemispheres.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F10"><?xmltex \currentcnt{10}?><?xmltex \def\figurename{Figure}?><label>Figure 10</label><caption><p id="d1e4751">Difference between total surface fluxes from the CAMS/INV-SRF data.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f10.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F11"><?xmltex \currentcnt{11}?><?xmltex \def\figurename{Figure}?><label>Figure 11</label><caption><p id="d1e4762">Difference between wetland surface fluxes from the CAMS/INV-SRF data.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f11.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F12"><?xmltex \currentcnt{12}?><?xmltex \def\figurename{Figure}?><label>Figure 12</label><caption><p id="d1e4774">Difference between other surface fluxes from the CAMS/INV-SRF data.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f12.png"/>

      </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F13"><?xmltex \currentcnt{13}?><?xmltex \def\figurename{Figure}?><label>Figure 13</label><caption><p id="d1e4785">Difference between total surface fluxes from the CAMS/INV-SRF-SAT data. No flux difference is available for 2022–2021, since the dataset currently ends in 2021.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f13.png"/>

      </fig>

      <p id="d1e4794">The agreement within 1<inline-formula><mml:math id="M280" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> of zonal growth rates derived from WFMD and CAMS/INV <inline-formula><mml:math id="M281" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data in Fig. <xref ref-type="fig" rid="Ch1.F8"/>, suggest that the structures observed in our zonal growth rates are not artifacts from sampling-related biases. However, we cannot rule out transport effects from this comparison, meaning we cannot clearly attribute changes in hemispheres or zonal bands over the years to a change in the source–sink<?pagebreak page588?> balance. Hence, we also investigated the change in surface fluxes between consecutive years which are readily available for the CAMS/INV data. In Figs. <xref ref-type="fig" rid="Ch1.F10"/>–<xref ref-type="fig" rid="Ch1.F12"/> we present total, wetland and non-wetland fluxes from CAMS/INV-SRF data, respectively. The category of non-wetland fluxes includes all other anthropogenic emissions as well as contributions from oceans, wild animals, the soil sink, termites, and biomass burning.</p>
      <p id="d1e4821">Large changes in fluxes are identified between all the years investigated. The wetland flux difference between 2019 and 2020 indicate a strong increase in the NH as indicated by <xref ref-type="bibr" rid="bib1.bibx38" id="text.75"/> as well as some increase in the SH wetlands as reported by <xref ref-type="bibr" rid="bib1.bibx19" id="text.76"/> and <xref ref-type="bibr" rid="bib1.bibx41" id="text.77"/>. We expect the SH wetland fluxes to be underestimated as indicated by <xref ref-type="bibr" rid="bib1.bibx19" id="text.78"/> because the CAMS/INV-SRF data is based on ground-based measurements from the NOAA network, similar to the inversion performed by <xref ref-type="bibr" rid="bib1.bibx38" id="text.79"/>, due to the poor coverage in the tropics. Interestingly, wetland fluxes from CAMS/INV-SRF-SAT data including satellite measurements from GOSAT show stronger SH wetland emissions between 2019 and 2020 as shown in Fig. <xref ref-type="fig" rid="Ch1.F13"/>. Additionally, an increase in non-wetland fluxes occurs between 2019–2020 and 2020–2021. In the first case these increases are mainly focused on China, while in the second case additional increases over the Indian subcontinent can be seen. Between 2021 and 2022 a clear decrease in total surface fluxes can be seen in large parts of the NH, while strong increases can be observed over the whole of South America. The large decreases in the NH can be clearly attributed to changes in the non-wetland fluxes, while the increase over South America seems to involve a combination of wetland and other fluxes. Therefore, CAMS/INV fluxes imply that the changes in zonal growth rates we observed both in WFMD and CAMS/INV are not merely due to changes in transport patterns but correlate with changes in surface methane fluxes between the years. This conclusion is strengthened by the qualitative agreement of the flux changes between CAMS/INV-SRF and the aforementioned studies by <xref ref-type="bibr" rid="bib1.bibx38" id="text.80"/>, <xref ref-type="bibr" rid="bib1.bibx19" id="text.81"/>, and <xref ref-type="bibr" rid="bib1.bibx41" id="text.82"/>. However, further research is needed to substantiate these inferences.</p>
</sec>
<sec id="Ch1.S7" sec-type="conclusions">
  <label>7</label><title>Conclusions</title>
      <p id="d1e4859">In this study, we presented a DLM-based approach to calculate methane growth rates and AMIs from S5P/TROPOMI data. We addressed sampling-related biases by comparing AMIs and growth rates derived from CAMS/INV <inline-formula><mml:math id="M282" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data both with and without S5P <inline-formula><mml:math id="M283" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> sampling. Further, we included a bias related to the model selection in our error budget. Our calculations of global AMIs based on WFMDv1.8 data from 2018 to 2022 demonstrate good agreement with other AMIs. Additionally, we separated the influence of the fitting method and the underlying data by applying our DLM approach to other datasets. We show that using the same input data results in agreement within 1<inline-formula><mml:math id="M284" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> between all AMIs. Using the same method but different input data results in qualitative agreement but differences larger than 1<inline-formula><mml:math id="M285" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>. Nevertheless, the consistency of AMIs derived from diverse datasets, such as ground-based data from NOAA and dry-air mole fraction data from WFMDv1.8 and UB–C3S–CAMS, highlights the robustness of these various approaches. The record methane increase in 2020 and 2021 is therefore well-identified in the different datasets, which use different methods to assess AMIs. The underlying factors driving these increases, as discussed in Sect. <xref ref-type="sec" rid="Ch1.S4"/>, remain however a subject of debate.</p>
      <p id="d1e4900">In addition to global AMIs, we investigated growth rates for 20<inline-formula><mml:math id="M286" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> zonal bands which provide spatial information to the global AMIs. We argue that this is possible due to (a) the faster zonal mixing in comparison to meridional mixing and (b) the faster satellite sampling in comparison to the meridional mixing times. Firstly, comparisons of zonal growth rates from S5P/TROPOMI data with growth rates from CAMS/INV-SRF <inline-formula><mml:math id="M287" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data show agreement within 1<inline-formula><mml:math id="M288" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>. Additionally, we investigated growth rates calculated from CAMS/INV-SRF <inline-formula><mml:math id="M289" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data filtered using a S5P <inline-formula><mml:math id="M290" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> mask which indicate that no significant sampling biases exist for the zonal band approach. Still, we want to emphasize that meridional transport can affect the zonal growth rates, meaning they do not necessarily indicate changes in the<?pagebreak page589?> sources and sinks of methane but might also show systematic changes in transport patterns. The zonal growth rates exhibit clear differences between the hemispheres for 2019 and 2022, whereas growth rates are more similar for 2020 and 2021. Differences within a hemisphere are mostly smaller and no additional short-term variations are visible, which might reflect the well-mixed state of the atmosphere within a hemisphere. The low growth rates in the SH in 2019 and the subsequent increases suggest a rise in atmospheric methane in that region possibly driven by tropical wetland emissions according to <xref ref-type="bibr" rid="bib1.bibx19" id="text.83"/>, <xref ref-type="bibr" rid="bib1.bibx41" id="text.84"/>, and <xref ref-type="bibr" rid="bib1.bibx53" id="text.85"/>. Other factors potentially contributing to these changes include variations in the OH sink due to pollutant reductions during the COVID-19 pandemic <xref ref-type="bibr" rid="bib1.bibx19 bib1.bibx41 bib1.bibx38" id="paren.86"/> and the changes in global methane emissions due to the COVID-19 pandemic and the subsequent recovery <xref ref-type="bibr" rid="bib1.bibx20" id="paren.87"/>.</p>
      <p id="d1e4968">We further investigated these inter-hemispheric differences by investigating the surface fluxes available from CAMS/INV data. We argue that this is possible since (a) growth rates derived from WFMDv1.8 data are similar to growth rates from CAMS/INV data and (b) no significant sampling bias is present, as we showed in Sect. <xref ref-type="sec" rid="Ch1.S3.SS4"/>. The total surface fluxes show clear changes between the years, and the partitioning into wetland and non-wetland (mainly anthropogenic) fluxes allows further interpretation. Furthermore, changes in fluxes show reasonable qualitative agreement with findings reported by <xref ref-type="bibr" rid="bib1.bibx19" id="text.88"/>, <xref ref-type="bibr" rid="bib1.bibx41" id="text.89"/>, and <xref ref-type="bibr" rid="bib1.bibx38" id="text.90"/>.</p>
      <p id="d1e4982">In addition to the confirmation of known results, new conclusions are also drawn. Most notably, the decrease in the global AMI in 2022 is caused by reduced NH zonal growth rates. This is clearly visible in zonal growth rates derived from S5P <inline-formula><mml:math id="M291" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and CAMS/INV <inline-formula><mml:math id="M292" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data. Investigation of the corresponding model surface fluxes indicates that changes in zonal growth rates are consistent with the decrease in non-wetland fluxes in the NH and the continuing increase in wetland fluxes in the SH. However, more research is needed to substantiate this inferred connection between the change in NH growth rates and fluxes.</p>
      <p id="d1e5008">In summary, our DLM-based approach allows calculation of growth rates or AMIs for global and zonal S5P/TROPOMI data. This approach is computationally inexpensive and readily allows for the constant integration of new data, enabling timely assessments of global methane concentration changes. Importantly, no additional prior information about the atmospheric state is required. We believe that our approach provides an additional valuable tool for investigating atmospheric methane concentrations, enabling rapid identification of regions of interest, such as the 2022 NH. Furthermore, our approach can be readily applied to other datasets facing similar challenges, such as inhomogeneous sampling, non-linear trends, and data gaps. For the 70–90<inline-formula><mml:math id="M293" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N band, our method failed to identify any changes in growth rates. However, this result is in good agreement with the growth rates from CAMS/INV-SRF <inline-formula><mml:math id="M294" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">XCH</mml:mi><mml:mn mathvariant="normal">4</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> data, which themselves only show small variations. This indicates that (a) the small changes in growth rates could not be distinguished from the random variability in the data or that (b) no anomalous increases in growth rates are visible for the northern high-latitude regions in the observed period from 2018 to 2022.</p>
      <p id="d1e5031">Future research could aim to improve this approach, especially for high-latitude regions, to identify smaller changes in growth rates. Better estimates of the impact of meridional transport on zonal growth rates could help to provide better error estimates for our method. The 2022 decrease in NH growth rates could be investigated in more detail and this approach be extended to include datasets of other atmospheric constituents. Data from future satellite missions, with lower uncertainties and increased data coverage, could enable the investigation of sub-annual changes in growth rates, which are presently not detectable. Finally, zonal growth rates of long-lived gases (e.g. HF) without any significant sources or sinks could possibly enable the quantification of atmospheric transport patterns.</p>
</sec>

      
      </body>
    <back><app-group>

<app id="App1.Ch1.S1">
  <?xmltex \currentcnt{A}?><label>Appendix A</label><title>Model set-up and ensemble size</title>
      <p id="d1e5045">The structure of our DLMs assumes that the measured methane signal can be separated into a slowly changing background level, a seasonal component and noise term. This section closely follows the more detailed description in <xref ref-type="bibr" rid="bib1.bibx17" id="text.91"/> and <xref ref-type="bibr" rid="bib1.bibx25" id="text.92"/>.</p>
      <p id="d1e5054">The level component can be described by the following formulas:

              <disp-formula specific-use="align" content-type="numbered"><mml:math id="M295" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="App1.Ch1.S1.E12"><mml:mtd><mml:mtext>A1</mml:mtext></mml:mtd><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mi>t</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mi>t</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mo>,</mml:mo><mml:mtext>level</mml:mtext></mml:mrow></mml:msub><mml:mo>,</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mo>,</mml:mo><mml:mtext>level</mml:mtext></mml:mrow></mml:msub><mml:mo>∼</mml:mo><mml:mi>N</mml:mi><mml:mfenced close=")" open="("><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>level</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mfenced><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="App1.Ch1.S1.E13"><mml:mtd><mml:mtext>A2</mml:mtext></mml:mtd><mml:mtd><mml:mstyle displaystyle="true" class="stylechange"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mi>t</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mo>,</mml:mo><mml:mtext>trend</mml:mtext></mml:mrow></mml:msub><mml:mo>,</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mo>,</mml:mo><mml:mtext>trend</mml:mtext></mml:mrow></mml:msub><mml:mo>∼</mml:mo><mml:mi>N</mml:mi><mml:mfenced close=")" open="("><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>trend</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mfenced><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

          <inline-formula><mml:math id="M296" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mi>t</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the level, <inline-formula><mml:math id="M297" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ν</mml:mi><mml:mi>t</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the trend (i.e. the slope or growth rate), and <inline-formula><mml:math id="M298" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mi>t</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> are steps in a random walk sampled from a Gaussian distribution. The random walks allow components to change over time. Since we want to allow for a smoothly changing level, we allow the trend to change over time. Additionally, we enforce a constraint of zero variance for the level to ensure that short-term fluctuations in the background level are not allowed:

              <disp-formula specific-use="align" content-type="numbered"><mml:math id="M299" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="App1.Ch1.S1.E14"><mml:mtd><mml:mtext>A3</mml:mtext></mml:mtd><mml:mtd><mml:mstyle class="stylechange" displaystyle="true"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>level</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>=</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="App1.Ch1.S1.E15"><mml:mtd><mml:mtext>A4</mml:mtext></mml:mtd><mml:mtd><mml:mstyle class="stylechange" displaystyle="true"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>trend</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula></p>
      <?pagebreak page590?><p id="d1e5296">The seasonal part of the signal is modelled by a truncated Fourier series with <inline-formula><mml:math id="M300" display="inline"><mml:mi>h</mml:mi></mml:math></inline-formula> harmonics:
          <disp-formula id="App1.Ch1.S1.E16" content-type="numbered"><label>A5</label><mml:math id="M301" display="block"><mml:mrow><mml:msub><mml:mi mathvariant="italic">γ</mml:mi><mml:mi>t</mml:mi></mml:msub><mml:mo>=</mml:mo><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>h</mml:mi></mml:munderover><mml:msub><mml:mi mathvariant="italic">γ</mml:mi><mml:mrow><mml:mi>j</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
        with<?xmltex \hack{\newpage}?>

              <disp-formula specific-use="gather" content-type="numbered"><mml:math id="M302" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="App1.Ch1.S1.E17"><mml:mtd><mml:mtext>A6</mml:mtext></mml:mtd><mml:mtd><mml:mrow><mml:mstyle class="stylechange" displaystyle="true"/><mml:mtable rowspacing="0.2ex" class="split" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd><mml:mrow><mml:msub><mml:mi mathvariant="italic">γ</mml:mi><mml:mrow><mml:mi>j</mml:mi><mml:mo>,</mml:mo><mml:mi>t</mml:mi><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msub><mml:mo>=</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mspace width="0.25em" linebreak="nobreak"/><mml:msub><mml:mi mathvariant="italic">γ</mml:mi><mml:mrow><mml:mi>j</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:mrow class="chem"><mml:mi mathvariant="normal">cos</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:msub><mml:mi mathvariant="italic">λ</mml:mi><mml:mi>j</mml:mi></mml:msub><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="italic">γ</mml:mi><mml:mrow><mml:mi>j</mml:mi><mml:mi>t</mml:mi></mml:mrow><mml:mo>∗</mml:mo></mml:msubsup><mml:mrow class="chem"><mml:mi mathvariant="normal">sin</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:msub><mml:mi mathvariant="italic">λ</mml:mi><mml:mi>j</mml:mi></mml:msub><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mtext>seas</mml:mtext></mml:msub><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mspace linebreak="nobreak" width="0.25em"/><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mtext>seas</mml:mtext></mml:msub><mml:mo>∼</mml:mo><mml:mi>N</mml:mi><mml:mfenced close=")" open="("><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>seas</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mfenced><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.25em"/><mml:mspace width="0.25em" linebreak="nobreak"/><mml:mspace width="0.25em" linebreak="nobreak"/><mml:mspace linebreak="nobreak" width="0.25em"/><mml:msub><mml:mi mathvariant="italic">λ</mml:mi><mml:mi>j</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mi mathvariant="italic">π</mml:mi><mml:mi>j</mml:mi></mml:mrow><mml:mi>s</mml:mi></mml:mfrac></mml:mstyle><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:mrow></mml:mtd></mml:mlabeledtr><mml:mlabeledtr id="App1.Ch1.S1.E18"><mml:mtd><mml:mtext>A7</mml:mtext></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:mtable class="split" rowspacing="0.2ex" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">γ</mml:mi><mml:mrow><mml:mi>j</mml:mi><mml:mo>,</mml:mo><mml:mi>t</mml:mi><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mo>∗</mml:mo></mml:msubsup><mml:mo>=</mml:mo></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mspace linebreak="nobreak" width="0.25em"/><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">γ</mml:mi><mml:mrow><mml:mi>j</mml:mi><mml:mi>t</mml:mi></mml:mrow></mml:msub><mml:mrow class="chem"><mml:mi mathvariant="normal">sin</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:msub><mml:mi mathvariant="italic">λ</mml:mi><mml:mi>j</mml:mi></mml:msub><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="italic">γ</mml:mi><mml:mrow><mml:mi>j</mml:mi><mml:mi>t</mml:mi></mml:mrow><mml:mo>∗</mml:mo></mml:msubsup><mml:mrow class="chem"><mml:mi mathvariant="normal">cos</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:msub><mml:mi mathvariant="italic">λ</mml:mi><mml:mi>j</mml:mi></mml:msub><mml:mo>)</mml:mo><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mtext>seas</mml:mtext><mml:mo>∗</mml:mo></mml:msubsup><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mspace linebreak="nobreak" width="0.25em"/><mml:msubsup><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mtext>seas</mml:mtext><mml:mo>∗</mml:mo></mml:msubsup><mml:mo>∼</mml:mo><mml:mi>N</mml:mi><mml:mfenced close=")" open="("><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>seas</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mfenced><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.25em"/><mml:mspace width="0.25em" linebreak="nobreak"/><mml:mspace linebreak="nobreak" width="0.25em"/><mml:mspace width="0.25em" linebreak="nobreak"/><mml:mi>j</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mi mathvariant="normal">…</mml:mi><mml:mo>,</mml:mo><mml:mi>h</mml:mi><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

          where <inline-formula><mml:math id="M303" display="inline"><mml:mi>s</mml:mi></mml:math></inline-formula> describes the seasonality of the data, e.g. for monthly data <inline-formula><mml:math id="M304" display="inline"><mml:mrow><mml:mi>s</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:math></inline-formula> or for daily data <inline-formula><mml:math id="M305" display="inline"><mml:mrow><mml:mi>s</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">365</mml:mn></mml:mrow></mml:math></inline-formula> when modelling yearly patterns. The value of <inline-formula><mml:math id="M306" display="inline"><mml:mrow><mml:mi>s</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">365.25</mml:mn></mml:mrow></mml:math></inline-formula> can be used to account for leap years. We use <inline-formula><mml:math id="M307" display="inline"><mml:mrow><mml:mi>s</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">365.2</mml:mn></mml:mrow></mml:math></inline-formula>, which is equal to the average number of days per year between 2018 and 2022. For <inline-formula><mml:math id="M308" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>seas</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">0</mml:mn></mml:mrow></mml:math></inline-formula> the seasonal cycle is allowed to change over time. We allow values of <inline-formula><mml:math id="M309" display="inline"><mml:mrow><mml:mi>h</mml:mi><mml:mo>∈</mml:mo><mml:mo mathvariant="italic">{</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">3</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">4</mml:mn><mml:mo mathvariant="italic">}</mml:mo></mml:mrow></mml:math></inline-formula> to account for varying levels of complexity in the seasonal cycle. The motivation for this is twofold. Firstly, we want to only model the basic structure of the seasonal cycle and not the whole signal. Secondly, the inclusion of more harmonics introduces further parameters which have to be estimated. This quickly leads to high uncertainties in the produced fit since not enough information is included in the data to account for the growing number of parameters.</p>

<?xmltex \floatpos{t}?><table-wrap id="App1.Ch1.S1.T4"><?xmltex \currentcnt{A1}?><label>Table A1</label><caption><p id="d1e5734">DLM parameters.</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="left"/>
     <oasis:colspec colnum="3" colname="col3" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Parameter</oasis:entry>
         <oasis:entry colname="col2">Description</oasis:entry>
         <oasis:entry colname="col3">Allowed range</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M312" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>level</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">Variability of the level</oasis:entry>
         <oasis:entry colname="col3">0</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M313" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>trend</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">Variability of the trend</oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M314" display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:mi mathvariant="normal">∞</mml:mi><mml:msup><mml:mo>]</mml:mo><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M315" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>seas</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">Variability of the seasonal cycle</oasis:entry>
         <oasis:entry colname="col3">0 or<inline-formula><mml:math id="M316" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M317" display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:mi mathvariant="normal">∞</mml:mi><mml:msup><mml:mo>]</mml:mo><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M318" display="inline"><mml:mi mathvariant="italic">ρ</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">Parameter of <inline-formula><mml:math id="M319" display="inline"><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M320" display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:msup><mml:mo>]</mml:mo><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M321" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">Variability of <inline-formula><mml:math id="M322" display="inline"><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col3"><inline-formula><mml:math id="M323" display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:mi mathvariant="normal">∞</mml:mi><mml:msup><mml:mo>]</mml:mo><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M324" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>irr</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">Variability of the Gaussian error</oasis:entry>
         <oasis:entry colname="col3">0 or<inline-formula><mml:math id="M325" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M326" display="inline"><mml:mrow><mml:mo>[</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:mi mathvariant="normal">∞</mml:mi><mml:msup><mml:mo>]</mml:mo><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M327" display="inline"><mml:mi>h</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">Number of harmonics</oasis:entry>
         <oasis:entry colname="col3">1–4<inline-formula><mml:math id="M328" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula></oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><table-wrap-foot><p id="d1e5737"><inline-formula><mml:math id="M310" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:math></inline-formula> Determined by maximum likelihood estimation during the DLM fit. <inline-formula><mml:math id="M311" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:math></inline-formula> Different settings are part of the ensemble.</p></table-wrap-foot><?xmltex \gdef\@currentlabel{A1}?></table-wrap>

      <p id="d1e6085">The noise term accounts for residual correlations as well as random Gaussian noise in the signal. Residual correlations can be modelled by an autoregressive component which includes a serial dependence between the observations. An autoregressive noise of order <inline-formula><mml:math id="M329" display="inline"><mml:mi>n</mml:mi></mml:math></inline-formula> includes a memory of the last <inline-formula><mml:math id="M330" display="inline"><mml:mi>n</mml:mi></mml:math></inline-formula> measurements. For <inline-formula><mml:math id="M331" display="inline"><mml:mrow><mml:mi>n</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>, this <inline-formula><mml:math id="M332" display="inline"><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> term is
          <disp-formula id="App1.Ch1.S1.E19" content-type="numbered"><label>A8</label><mml:math id="M333" display="block"><mml:mrow><?xmltex \hack{\hbox\bgroup\fontsize{9.5}{9.5}\selectfont$\displaystyle}?><mml:msub><mml:mi mathvariant="italic">η</mml:mi><mml:mrow><mml:mi>t</mml:mi><mml:mo>+</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mi mathvariant="italic">ρ</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:msub><mml:mi mathvariant="italic">η</mml:mi><mml:mi mathvariant="normal">t</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:msub><mml:mo>,</mml:mo><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:msub><mml:mo>∼</mml:mo><mml:mi>N</mml:mi><mml:mfenced open="(" close=")"><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mfenced><mml:mo>,</mml:mo><mml:mi mathvariant="italic">ρ</mml:mi><mml:mo>∈</mml:mo><mml:mo>[</mml:mo><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>]</mml:mo><mml:mo>,</mml:mo><?xmltex \hack{$\egroup}?></mml:mrow></mml:math></disp-formula>
        where <inline-formula><mml:math id="M334" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">η</mml:mi><mml:mi>t</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is the autoregressive component, <inline-formula><mml:math id="M335" display="inline"><mml:mi mathvariant="italic">ρ</mml:mi></mml:math></inline-formula> determines the strength of the autocorrelation (the memory of the previous time step), and <inline-formula><mml:math id="M336" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is again a step in a Gaussian random walk. This component introduces the parameters <inline-formula><mml:math id="M337" display="inline"><mml:mi mathvariant="italic">ρ</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M338" display="inline"><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:math></inline-formula> to the model. We confine our autoregressive component to the order of <inline-formula><mml:math id="M339" display="inline"><mml:mrow><mml:mi>n</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula>, which is enough to model the residual correlations in our data. Higher orders would introduce further parameters to be estimated and lead to a harder interpretability of the results. However, exclusion of the <inline-formula><mml:math id="M340" display="inline"><mml:mrow><mml:mrow class="chem"><mml:mi mathvariant="normal">AR</mml:mi></mml:mrow><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> component leads to bad fits since the model fails to account for the data variability.</p>
      <p id="d1e6325">An additional Gaussian noise can be included:
          <disp-formula id="App1.Ch1.S1.E20" content-type="numbered"><label>A9</label><mml:math id="M341" display="block"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mtext>irr</mml:mtext></mml:msub><mml:mo>,</mml:mo><mml:mspace width="0.25em" linebreak="nobreak"/><mml:mspace linebreak="nobreak" width="0.25em"/><mml:mspace linebreak="nobreak" width="0.25em"/><mml:mspace linebreak="nobreak" width="0.25em"/><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mtext>irr</mml:mtext></mml:msub><mml:mo>∼</mml:mo><mml:mi>N</mml:mi><mml:mfenced open="(" close=")"><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mtext>irr</mml:mtext><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mfenced><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula>
        We call this the <italic>irregular</italic> component.</p>
      <p id="d1e6372">The complete signal can then be written as the sum of these components:
          <disp-formula id="App1.Ch1.S1.E21" content-type="numbered"><label>A10</label><mml:math id="M342" display="block"><mml:mrow><mml:msub><mml:mi>y</mml:mi><mml:mi>t</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:msub><mml:mi mathvariant="italic">μ</mml:mi><mml:mi>t</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">γ</mml:mi><mml:mi>t</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">η</mml:mi><mml:mi>t</mml:mi></mml:msub><mml:mo>+</mml:mo><mml:msub><mml:mi mathvariant="italic">ϵ</mml:mi><mml:mtext>irr</mml:mtext></mml:msub><mml:mo>.</mml:mo></mml:mrow></mml:math></disp-formula></p>
      <p id="d1e6415">The ensemble size is determined by the number of possible model configurations. In our case this is determined by whether to allow variability of the seasonal cycle or whether to include a Gaussian error term and the number of harmonics: <inline-formula><mml:math id="M343" display="inline"><mml:mrow><mml:mi>N</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mo>⋅</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mo>⋅</mml:mo><mml:mn mathvariant="normal">4</mml:mn><mml:mo>=</mml:mo><mml:mn mathvariant="normal">16</mml:mn></mml:mrow></mml:math></inline-formula>. An overview of all the parameters can be found in Table <xref ref-type="table" rid="App1.Ch1.S1.T4"/>.</p>
</app>

<app id="App1.Ch1.S2">
  <?xmltex \currentcnt{B}?><label>Appendix B</label><title>Replication of complete NOAA GML and UB–C3S AMIs</title>
      <p id="d1e6452">To investigate the effect of the fitting method on AMIs we replicated AMIs calculated by the NOAA–GML and C3S in Figs. <xref ref-type="fig" rid="App1.Ch1.S2.F14"/> and <xref ref-type="fig" rid="App1.Ch1.S2.F15"/>, respectively. Here we present the comparison for the whole available time range (a subset of data can be seen in Table <xref ref-type="table" rid="Ch1.T3"/>).</p>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.S2.F14"><?xmltex \currentcnt{B1}?><?xmltex \def\figurename{Figure}?><label>Figure B1</label><caption><p id="d1e6463">Comparison of global annual methane increases derived from the NOAA–GML MBLR data using different methods.</p></caption>
        <?xmltex \hack{\textwidth\hsize}?>
        <?xmltex \igopts{width=227.622047pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f14.png"/>

      </fig>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.S2.F15"><?xmltex \currentcnt{B2}?><?xmltex \def\figurename{Figure}?><label>Figure B2</label><caption><p id="d1e6476">Comparison of global annual methane increases derived from C3S XCH4_OBS4MIPS v4.4 data which are extended by CAMS NRT data after 2021  using different methods.</p></caption>
        <?xmltex \hack{\textwidth\hsize}?>
        <?xmltex \igopts{width=227.622047pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f15.png"/>

      </fig>

<?xmltex \hack{\newpage}?>
</app>

<?pagebreak page591?><app id="App1.Ch1.S3">
  <?xmltex \currentcnt{C}?><label>Appendix C</label><title>Global AMIs and zonal growth rates derived from CAMS global inversion-optimized greenhouse concentrations</title>
      <p id="d1e6497">Here we present global AMIs and zonal growth rates for CAMS/INV-SRF-SAT data which includes satellite measurements from GOSAT in its optimization (see Figs. <xref ref-type="fig" rid="App1.Ch1.S3.F16"/> and <xref ref-type="fig" rid="App1.Ch1.S3.F17"/>).</p>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.S3.F16"><?xmltex \currentcnt{C1}?><?xmltex \def\figurename{Figure}?><label>Figure C1</label><caption><p id="d1e6506">Global annual methane increases derived from CAMS global inversion-optimized greenhouse concentrations including both surface and satellite observations.</p></caption>
        <?xmltex \igopts{width=207.705118pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f16.png"/>

      </fig>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.S3.F17"><?xmltex \currentcnt{C2}?><?xmltex \def\figurename{Figure}?><label>Figure C2</label><caption><p id="d1e6517">Zonal growth rates for 20<inline-formula><mml:math id="M344" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> bands derived from <bold>(a)</bold> Sentinel-5P TROPOMI WFMDv1.8 data and <bold>(b)</bold> CAMS/INV-SRF-SAT data. The errors show the 1<inline-formula><mml:math id="M345" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula> uncertainty.</p></caption>
        <?xmltex \hack{\textwidth\hsize}?>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f17.png"/>

      </fig>

<?xmltex \hack{\newpage}?>
</app>

<app id="App1.Ch1.S4">
  <?xmltex \currentcnt{D}?><label>Appendix D</label><title>WFMDv1.8 data coverage</title>
      <p id="d1e6560">Figure <xref ref-type="fig" rid="App1.Ch1.S4.F18"/> shows the area-normalized coverage of S5P/TROPOMI WFMDv1.8 data. It can be seen that the tropics, mid-latitudes, and high latitudes mostly have an average coverage of about 25 %, while the high-latitude regions have seasonal gaps due to the polar night.</p>

      <?xmltex \floatpos{h!}?><fig id="App1.Ch1.S4.F18"><?xmltex \currentcnt{D1}?><?xmltex \def\figurename{Figure}?><label>Figure D1</label><caption><p id="d1e6567">Area-normalized coverage of S5P/TROPOMI WFMDv1.8 data for 30<inline-formula><mml:math id="M346" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> zonal bands, representing the high-latitude, mid-latitude, and tropical regions. For the calculation, data on a 2<inline-formula><mml:math id="M347" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> <inline-formula><mml:math id="M348" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> 2<inline-formula><mml:math id="M349" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> grid were used. The coverage is given on a scale from 0 to 1, where 1 represents complete coverage within a band.</p></caption>
        <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://acp.copernicus.org/articles/24/577/2024/acp-24-577-2024-f18.png"/>

      </fig>

<?xmltex \hack{\newpage}?>
</app>
  </app-group><notes notes-type="codedataavailability"><title>Code and data availability</title>

      <p id="d1e6616">CAMS global inversion-optimized greenhouse gas fluxes and concentrations are available from <uri>https://ads.atmosphere.copernicus.eu/</uri> (last access: 21 June 2023, <xref ref-type="bibr" rid="bib1.bibx44" id="altparen.93"/>). Sentinel-5P TROPOMI WFMD data are available from <uri>https://www.iup.uni-bremen.de/carbon_ghg/products/tropomi_wfmd/</uri> (last access: 28 March 2023, <xref ref-type="bibr" rid="bib1.bibx43" id="altparen.94"/>). NOAA MBL data are available from <uri>https://gml.noaa.gov/ccgg/mbl/</uri> (last access: 30 October 2023, <xref ref-type="bibr" rid="bib1.bibx16" id="altparen.95"/>). Example code to recreate Fig. <xref ref-type="fig" rid="Ch1.F5"/> (global annual methane increases), including the gridding and processing of the data, is available at <ext-link xlink:href="https://doi.org/10.5281/zenodo.8178927" ext-link-type="DOI">10.5281/zenodo.8178927</ext-link> <xref ref-type="bibr" rid="bib1.bibx23" id="paren.96"/>.</p>
  </notes><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e6649">JH developed the methodology and conducted the formal analysis. OS provided information on the WFMDv1.8 data. MiB provided information on the UB–C3S–CAMS data. JPB provided valuable input on atmospheric transport effects. MaB provided supervision and helped with the conceptualization. JH wrote the initial draft of this paper. All the authors contributed significantly to the conception of the analysis, jointly discussed the results, and provided constructive comments to improve the manuscript.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e6656">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="d1e6662">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. While Copernicus Publications makes every effort to include appropriate place names, the final responsibility lies with the authors.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e6668">This publication uses and contains  modified Copernicus Atmosphere Monitoring Service information (2018–2022) and modified Copernicus Sentinel data (2018–2023). Sentinel-5 Precursor is an ESA mission implemented on behalf of the European Commission. The TROPOMI payload is a joint development by the European Space Agency (ESA) and the Netherlands Space Office (NSO). The Sentinel-5 Precursor ground-segment development has been funded by the ESA and with national contributions from the Netherlands, Germany, and Belgium. The pre-operational TROPOMI data processing was carried out on the Dutch national e-infrastructure with the support of the SURF cooperative. Scientific colour maps <xref ref-type="bibr" rid="bib1.bibx13" id="paren.97"/> are used in this study to prevent visual distortion of data and exclusion of readers with colour-vision deficiencies <xref ref-type="bibr" rid="bib1.bibx14" id="paren.98"/>.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e6679">This project is funded by the State and University of Bremen. In particular, the University of Bremen funding for the junior research group “Greenhouse gases in the Arctic” is acknowledged by Jonas Hachmeister and Michael Buchwitz. We gratefully acknowledge the funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation), grant no. 268020496 – TRR 172, within the Transregional Collaborative Research Center “ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)<inline-formula><mml:math id="M350" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:math></inline-formula>”. We also acknowledge the received funding from the ESA via projects GHG-CCI+ and MethaneCAMP (ESA contract nos. 4000126450/19/I-NB and 4000137895/22/I-AG) and from the German Ministry of Education and Research (BMBF) within its ITMS project via grant no. 01 LK2103A. The TROPOMI/WFMD version 1.8 data have been generated using funding from the ESA (GHG-CCI and MethaneCAMP projects). The TROPOMI/WFMD retrievals presented here were performed at HPC facilities of the IUP, University of Bremen, funded under DFG/FUGG grant nos. INST 144/379-1 and INST 144/493-1. Some of the AMIs presented were generated for Copernicus ESOTC 2022 (<uri>https://climate.copernicus.eu/climate-indicators/greenhouse-gas-concentrations</uri>, last access: 30 June 2023) funded by the EU Copernicus Climate Change Service via project no. C3S2_ 312a_Lot2. <?xmltex \hack{\newline}?><?xmltex \hack{\newline}?> The article processing charges for this open-access<?xmltex \notforhtml{\newline}?> publication were covered by the University of Bremen.</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e6702">This paper was edited by Bryan N. Duncan and reviewed by two anonymous referees.</p>
  </notes><ref-list>
    <title>References</title>

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