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  <front>
    <journal-meta><journal-id journal-id-type="publisher">GMD</journal-id><journal-title-group>
    <journal-title>Geoscientific Model Development</journal-title>
    <abbrev-journal-title abbrev-type="publisher">GMD</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">Geosci. Model Dev.</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">1991-9603</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/gmd-13-5813-2020</article-id><title-group><article-title>PMIF v1.0: assessing the potential of satellite observations to constrain <inline-formula><mml:math id="M1" 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> emissions from large cities and point sources<?xmltex \hack{\break}?> over the globe using synthetic data</article-title><alt-title>Potential of satellite observations to constrain CO<inline-formula><mml:math id="M2" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula> emissions</alt-title>
      </title-group><?xmltex \runningtitle{Potential of satellite observations to constrain CO${}_{2}$ emissions}?><?xmltex \runningauthor{Y.~Wang et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1 aff2">
          <name><surname>Wang</surname><given-names>Yilong</given-names></name>
          <email>wangyil@igsnrr.ac.cn</email>
        <ext-link>https://orcid.org/0000-0001-7176-2692</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Broquet</surname><given-names>Grégoire</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Bréon</surname><given-names>François-Marie</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-2128-739X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1 aff3">
          <name><surname>Lespinas</surname><given-names>Franck</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <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" rid="aff4">
          <name><surname>Reuter</surname><given-names>Maximilian</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-9141-3895</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>Meijer</surname><given-names>Yasjka</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff5">
          <name><surname>Loescher</surname><given-names>Armin</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-1218-2580</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff6">
          <name><surname>Janssens-Maenhout</surname><given-names>Greet</given-names></name>
          
        <ext-link>https://orcid.org/0000-0002-9335-0709</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Zheng</surname><given-names>Bo</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-8344-3445</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Ciais</surname><given-names>Philippe</given-names></name>
          
        </contrib>
        <aff id="aff1"><label>1</label><institution>Laboratoire des Sciences du Climat et de l'Environnement,
CEA-CNRS-UVSQ- Université Paris Saclay, 91191, Gif-sur-Yvette CEDEX,
France</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>Key Laboratory of Land Surface Pattern and Simulation, Institute of
Geographic Sciences and Natural Resources Research, Chinese Academy of
Sciences, Beijing, China</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Canadian Centre for Meteorological and Environmental Prediction, 2121 Transcanada Highway,<?xmltex \hack{\break}?> Dorval, QC, H9P 1J3, Canada</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>Institute of Environmental Physics (IUP), University of Bremen FB1,
Otto Hahn Allee 1, 28334 Bremen, Germany</institution>
        </aff>
        <aff id="aff5"><label>5</label><institution>European Space Agency (ESA), Noordwijk, the Netherlands</institution>
        </aff>
        <aff id="aff6"><label>6</label><institution>European Commission, Joint Research Centre, Directorate Sustainable
Resources, via E. Fermi 2749<?xmltex \hack{\break}?> (T.P. 123), 21027 Ispra, Italy</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Yilong Wang (wangyil@igsnrr.ac.cn)</corresp></author-notes><pub-date><day>26</day><month>November</month><year>2020</year></pub-date>
      
      <volume>13</volume>
      <issue>11</issue>
      <fpage>5813</fpage><lpage>5831</lpage>
      <history>
        <date date-type="received"><day>14</day><month>November</month><year>2019</year></date>
           <date date-type="rev-request"><day>2</day><month>January</month><year>2020</year></date>
           <date date-type="rev-recd"><day>20</day><month>September</month><year>2020</year></date>
           <date date-type="accepted"><day>8</day><month>October</month><year>2020</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2020 Yilong Wang et al.</copyright-statement>
        <copyright-year>2020</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://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020.html">This article is available from https://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020.html</self-uri><self-uri xlink:href="https://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020.pdf">The full text article is available as a PDF file from https://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020.pdf</self-uri>
      <abstract><title>Abstract</title>
    <p id="d1e232">This study assesses the potential of satellite imagery of vertically integrated columns of dry-air mole fractions of <inline-formula><mml:math id="M3" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> (<inline-formula><mml:math id="M4" 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>) to constrain the emissions from cities and power plants (called emission clumps) over the whole globe during 1 year. The imagery is simulated for one imager of the Copernicus mission on Anthropogenic Carbon Dioxide Monitoring (CO2M) planned by the European Space Agency and the European Commission. The width of the swath of the CO2M instruments is about
300 km and the ground horizontal resolution is about 2 km resolution. A
Plume Monitoring Inversion Framework (PMIF) is developed, relying on a
Gaussian plume model to simulate the <inline-formula><mml:math id="M5" 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> plumes of each emission clump and on a combination of overlapping assimilation windows to solve for the inversion problem. The inversion solves for the 3 h mean emissions (during 08:30–11:30 local time) before satellite overpasses and for the mean emissions during other hours of the day (over the aggregation between
00:00–08:30 and 11:30–00:00) for each clump and for the 366 d of the year. Our analysis focuses on the derivation of the uncertainty in the inversion estimates (the “posterior uncertainty”) of the clump emissions. A comparison of the results obtained with PMIF and those from a previous study using a complex 3-D Eulerian transport model for a single city (Paris) shows that the PMIF system provides the correct order of magnitude for the uncertainty reduction of emission estimates (i.e., the relative difference between the prior and posterior uncertainties). Beyond the one city or few large cities studied by previous studies, our results provide, for the first time, the global statistics of the uncertainty reduction of emissions for the full range of global clumps (differing in emission rate and spread, and distance from other major clumps) and meteorological conditions. We show that only the clumps with an annual emission budget higher than 2 MtC yr<inline-formula><mml:math id="M6" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> can potentially have their emissions between 08:30 and 11:30 constrained with a posterior uncertainty smaller than 20 % for more than 10 times within 1 year (ignoring the potential to cross or extrapolate information between 08:30–11:30 time windows on different days). The PMIF inversion results are also aggregated in time to investigate the potential of CO2M observations to constrain daily and annual emissions, relying on the extrapolation of information obtained for 08:30–11:30 time<?pagebreak page5814?> windows during days when clouds and aerosols do not mask the plumes, based on various assumptions regarding the temporal auto-correlations of the uncertainties in the emission estimates that are used as a prior knowledge in the Bayesian framework of PMIF. We show that the posterior uncertainties of daily and annual emissions are highly dependent on these temporal auto-correlations, stressing the need for systematic assessment of the sources of uncertainty in the
spatiotemporally resolved emission inventories used as prior estimates in
the inversions. We highlight the difficulty in constraining the total budget of
<inline-formula><mml:math id="M7" 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> emissions from all the cities and power plants within a country or over the globe with satellite <inline-formula><mml:math id="M8" 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> measurements only, and calls for integrated inversion systems that exploit multiple types of measurements.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e312">Cities, thermal power plants and industrial factories cover a very small fraction of the land surface but are emitting a large amount of <inline-formula><mml:math id="M9" 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>. Many cities and regions are taking actions to reduce their greenhouse gas emissions. However, there are large uncertainties in the estimate of emissions from these <inline-formula><mml:math id="M10" 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> hotspots (Gately and Hutyra, 2017; Gurney et al., 2016). In addition, emissions at high temporal resolution (e.g., daily and hourly) depend on socio-economic activity and climate fluctuations and thus have large variability. The large uncertainties and fluctuations of emissions at local scale have raised
a growing political and scientific interest for an accurate and continuous
monitoring of these local <inline-formula><mml:math id="M11" 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> emissions based on atmospheric
measurements (Duren and Miller, 2012).</p>
      <p id="d1e348">Measurements of <inline-formula><mml:math id="M12" 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> mole fractions from in situ surface networks,
aircraft campaigns and mobile platforms around cities (Bréon et al., 2015; Lauvaux et al., 2016; Staufer et al., 2016) have been used to
characterize the <inline-formula><mml:math id="M13" 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> signals downwind of large cities and to quantify the underlying emissions based on an atmospheric inversion approach. However,
such urban networks are deployed for a few cities only. Alternatively,
vertically integrated columns of dry-air mole fractions of <inline-formula><mml:math id="M14" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>
<inline-formula><mml:math id="M15" display="inline"><mml:mrow class="chem"><mml:mo>(</mml:mo><mml:msub><mml:mi mathvariant="normal">XCO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>) from satellites offer the opportunity to sample the atmosphere
with global coverage. Kort et al. (2012) and Janardanan (2016) found that
significant <inline-formula><mml:math id="M16" 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> enhancements could be detected over some megacities
using Greenhouse Gases Observing Satellite (GOSAT) <inline-formula><mml:math id="M17" 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> observations.
Schwandner et al. (2017) also found <inline-formula><mml:math id="M18" 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> enhancements of 4.4 to 6.1 ppm in the Los Angeles urban <inline-formula><mml:math id="M19" 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> dome using observations from the Orbiting Carbon Observatory-2 (OCO-2). Nassar et al. (2017) used the <inline-formula><mml:math id="M20" 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> observations from OCO-2 to quantify <inline-formula><mml:math id="M21" 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> emissions from several medium- to large-sized coal power plants. However, the design of GOSAT and OCO-2 observations with sparse sampling was mainly focused on the monitoring of <inline-formula><mml:math id="M22" 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> natural fluxes. Recent studies show a limited amount of clear detections of transects of <inline-formula><mml:math id="M23" 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> plumes from cities or plants in OCO-2 observations (Zheng et al., 2020) so that GOSAT and OCO-2 data keep on being hardly used to estimate <inline-formula><mml:math id="M24" 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> city emissions. The potential for reducing uncertainties in <inline-formula><mml:math id="M25" 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> emissions at the scale of point sources (Bovensmann et al., 2010), cities (Broquet et al., 2018; Pillai et al., 2016) and agglomerations of several cities (O'Brien et al., 2016) should dramatically change with the planned satellite missions with imaging
capabilities. These studies consistently showed that imaging capability with
a wide swath (typically on the order of 200–300 km), a high resolution
(<inline-formula><mml:math id="M26" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>–3 km horizontal resolution) and a high single sounding precision (<inline-formula><mml:math id="M27" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> ppm) are required for satellite <inline-formula><mml:math id="M28" 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> measurements for the monitoring of <inline-formula><mml:math id="M29" display="inline"><mml:mrow class="chem"><mml:msub><mml:mi mathvariant="normal">CO</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> emissions from large point sources and cities. Several satellite <inline-formula><mml:math id="M30" 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> imagery concepts have been proposed: (i) the OCO-3 NASA (National Aeronautics and Space Administration) mission which has been installed on the International Space Station (ISS) in May 2019; (ii) the CarbonSat mission which was a candidate for the European Space Agency's (ESA's) Earth Explorer 8 opportunity (Bovensmann et al., 2015) but was not selected; (iii) the “city-mode” of the MicroCarb mission of the Centre National d'Etudes Spatiales (CNES), which should be launched in 2021 (Bertaux et al., 2019); (iv) the GeoCARB geostationary mission which was selected as the Earth Venture Mission-2 by NASA; and (v) the Copernicus Anthropogenic Carbon Dioxide Monitoring (CO2M) mission consisting of a constellation of <inline-formula><mml:math id="M31" 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> imagers that is currently studied by the ESA on behalf of the European Commission in the context of the European Union Copernicus programme. This CO2M satellite constellation is a crucial element that will contribute to the operational anthropogenic <inline-formula><mml:math id="M32" 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> monitoring and verification support capacity currently under development by the European Commission with support from the ESA, European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT) and the European Centre
for Medium-Range Weather Forecasts (ECMWF) (Ciais et al., 2015; Pinty et al., 2017, 2019).</p>
      <?pagebreak page5815?><p id="d1e585">The main approach currently investigated for the estimate of <inline-formula><mml:math id="M33" 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>
emissions from satellite <inline-formula><mml:math id="M34" 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> images consists of identifying the
<inline-formula><mml:math id="M35" 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> plumes downwind of the main <inline-formula><mml:math id="M36" 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> emission sources. The size of the plumes and the magnitude of <inline-formula><mml:math id="M37" 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> enhancements in these plumes are tightly linked to the emissions. Wang et al. (2019) developed an
algorithm to extract, from gridded emission maps, a conservative set of area
(cities) and point sources (power plants) with intense emissions around the
globe which can generate coherent <inline-formula><mml:math id="M38" 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> plumes that may be observed from space, given the precision of current satellite observations. This set was conservative because it is inferred for idealized meteorological condition without wind. These emitting sources were called “emission clumps”. Wang et al. (2019) identified 11 314 individual clumps which contribute 72 % of the global fossil fuel <inline-formula><mml:math id="M39" 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> emissions from the ODIAC (Open-source Data Inventory for Anthropogenic <inline-formula><mml:math id="M40" 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> version 2017; Oda et al., 2018) 1 km resolution inventory.</p>
      <p id="d1e677">Broquet et al. (2018) showed that the part of the <inline-formula><mml:math id="M41" 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> plumes exploited by the atmospheric inversion in satellite images corresponds to a few hours of the clump emissions before the satellite overpass. The <inline-formula><mml:math id="M42" 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> signature of the earlier clump emissions is too diluted to be filtered from the measurement errors and the signature of other <inline-formula><mml:math id="M43" 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> sources and sinks. Further, emissions from a given clump vary in time during the day, for instance due to the variations of traffic in cities (Yang et al., 2019), from day to day and between seasons, with more emissions associated with heating in winter over cold regions (Bréon et al., 2017). Therefore, the estimate of annual budgets of the clump emissions based on satellite observation during daytime (generally for a fixed local time since most of the missions use heliosynchronous orbits) and for low cloud coverage is a challenge and cannot rely on the direct information from the satellite imagery. It relies on the extrapolation of information from the time windows for which the emissions are well constrained. Such an extrapolation is based on the correlation of the uncertainty in emissions in time, and more precisely, in the atmospheric inversion framework, on the temporal auto-correlations of the uncertainty in the inventories used as a prior knowledge by the Bayesian framework of the inversion (see Sect. 2.6).</p>
      <p id="d1e714">Previous studies on the potential of the satellite <inline-formula><mml:math id="M44" 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> imagery to
constrain the emissions from clumps were limited to a single target or a few large
targets, such as power plants in Bovensmann et al. (2010), Berlin in Pillai et al. (2016) and in Kuhlmann et al. (2019), and Paris in Broquet et al. (2018). However, much of the global <inline-formula><mml:math id="M45" 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> emissions occur in smaller cities and plants. The potential and design of satellite missions dedicated to the monitoring of the <inline-formula><mml:math id="M46" 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> emissions like CO2M needs to be assessed for a much more representative range of sources over the whole globe. The inversion framework used by Pillai et al. (2016) and
Broquet et al. (2018) were based on full 3-D Eulerian atmospheric transport models at high spatial resolution (on the order of 2 km). Such inversions are much too expensive in terms of computation cost to be applied in a systematic way to the full set of clumps across the globe.</p>
      <p id="d1e750">Therefore, in this study, we develop a Plume Monitoring Inversion Framework
(PMIF) and conduct a set of observing system simulation experiments (OSSEs)
to assess, for the first time, the performance of a satellite instrument to
monitor the emissions of all the clumps across the globe and over a whole
year. The imager studied has the foreseen characteristics of the individual
satellites of the forthcoming CO2M mission. It would be a high-resolution
spectrometer, with <inline-formula><mml:math id="M47" display="inline"><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula> resolution pixels and a swath of 300 km, and it would be placed on a Sun-synchronous orbit ensuring global coverage in 4 d. The PMIF inversion system relies on the list of clumps extracted by Wang et al. (2019) from the ODIAC inventory, on the Gaussian plume model to simulate the <inline-formula><mml:math id="M48" 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> plumes generated by the emissions from these clumps, on an analytical inverse modeling framework, and on a combination of overlapping assimilation windows to solve for the inversion problem over the globe and a full year. It also addresses the question of temporal extrapolation that is needed to generate estimates of annual emissions from the information of a limited number of time windows for which emissions are well constrained by the direct satellite images, by accounting for the temporal auto-correlation of the prior uncertainties. The performance is assessed in terms of the uncertainties in the emissions (Sect. 2.1) at different scales. The PMIF uses a Gaussian plume model at the local scale to ensure that the computation cost is affordable. Such a model can often hardly fit with actual plumes over the distances considered in this study (due to variations in the wind field, topography, vertical mixing etc. over such distances) but is shown, when driven with suitable parameters, to provide a satisfactory simulation of the plume extent and amplitudes, which appear to be the main drivers of the targeted computations of uncertainties in the emissions in our OSSE framework (as shown in Sect. 3.1). In PMIF, we also ignore the impact of some sources of uncertainties on the inversion of emissions, including systematic errors in the <inline-formula><mml:math id="M49" 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> retrievals, the impact of uncertainties in diffuse anthropogenic emissions outside clumps and in
non-fossil <inline-formula><mml:math id="M50" 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> fluxes (within and outside clumps), and in the spatial
and temporal variations of emissions within the clump and in the short time
windows that the inversion aims to solve. These impacts are discussed in
detail afterwards.</p>
      <p id="d1e806">This PMIF system provides an indication of the satellite system capabilities
for the full range of cities and power plants varying in topography,
emission budget and spread, proximity to other major sources, and for a
large range of meteorological conditions. It complements other systems that
focus on specific regions with more complex (but area-limited) models and
consideration of diffuse sources and natural fluxes, allowing for
extrapolating and up-scaling results of those more complex systems to get a
more systematic understanding of their implications for the monitoring of
<inline-formula><mml:math id="M51" 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> emissions from all detectible clumps over the globe.</p>
      <p id="d1e820">The PMIF system and the OSSEs analyzed in this first study are described in
Sect. 2. The results obtained with the PMIF for the city of Paris are
compared with those of Broquet et al. (2018) in Sect. 3.1. The uncertainty in the retrieved emissions of individual clumps with one imaging satellite for 3 h time windows, for daily emissions and for annual emissions is assessed in Sect. 3.2–3.4. Section 4 discusses the drivers of the spatial variations of the uncertainty in the retrieved emissions, the limitations of PMIF and the implications for a future operational observing system.</p>
</sec>
<?pagebreak page5816?><sec id="Ch1.S2">
  <label>2</label><title>Methodology</title>
<sec id="Ch1.S2.SS1">
  <label>2.1</label><title>Plume Monitoring Inversion Framework</title>
      <p id="d1e838">The theoretical framework of the inversion system developed in this study is
the same as the traditional atmospheric inversions. The inversion derives a
statistical estimate for a set of control variables <inline-formula><mml:math id="M52" display="inline"><mml:mi mathvariant="bold-italic">x</mml:mi></mml:math></inline-formula> in a model <inline-formula><mml:math id="M53" display="inline"><mml:mrow><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mo>→</mml:mo><mml:mi mathvariant="bold-italic">y</mml:mi><mml:mo>=</mml:mo><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="bold-italic">x</mml:mi></mml:mrow></mml:math></inline-formula> that simulates the satellite <inline-formula><mml:math id="M54" 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> measurements <inline-formula><mml:math id="M55" display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="bold-italic">y</mml:mi><mml:mi mathvariant="normal">o</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula>. The model <inline-formula><mml:math id="M56" display="inline"><mml:mi mathvariant="bold">M</mml:mi></mml:math></inline-formula> linking <inline-formula><mml:math id="M57" display="inline"><mml:mi mathvariant="bold-italic">x</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M58" display="inline"><mml:mi mathvariant="bold-italic">y</mml:mi></mml:math></inline-formula> is a combination of flux and atmospheric transport models (detailed in Sect. 2.4) and is called observation operator hereafter. As explained below, we do not have a constant term added to <inline-formula><mml:math id="M59" display="inline"><mml:mrow><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="bold-italic">x</mml:mi></mml:mrow></mml:math></inline-formula> in the observation operator of the PMIF that would gather the atmospheric <inline-formula><mml:math id="M60" 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> signature of the fluxes not controlled by the inversion (like non-fossil fluxes and the background <inline-formula><mml:math id="M61" 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> field) since the uncertainty in such fluxes is ignored. The inversion follows a Bayesian statistical framework, updating the statistical prior estimate of <inline-formula><mml:math id="M62" display="inline"><mml:mi mathvariant="bold-italic">x</mml:mi></mml:math></inline-formula> based on the statistical information from the assimilation of <inline-formula><mml:math id="M63" 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> measurements <inline-formula><mml:math id="M64" display="inline"><mml:mi mathvariant="bold-italic">y</mml:mi></mml:math></inline-formula> into the observation operator. The distributions of the prior estimate and of the misfits between the actual observations <inline-formula><mml:math id="M65" display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="bold-italic">y</mml:mi><mml:mi mathvariant="normal">o</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula> and simulated ones due to errors in the observations and in the observation operator (called the “observation errors”) are assumed to be unbiased and to have the Gaussian forms <inline-formula><mml:math id="M66" display="inline"><mml:mrow><mml:mi>N</mml:mi><mml:mo>(</mml:mo><mml:msup><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mi mathvariant="normal">b</mml:mi></mml:msup><mml:mo>,</mml:mo><mml:mi mathvariant="bold">B</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M67" display="inline"><mml:mrow><mml:mi>N</mml:mi><mml:mo>(</mml:mo><mml:mn mathvariant="bold">0</mml:mn><mml:mo>,</mml:mo><mml:mi mathvariant="bold">R</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, where <inline-formula><mml:math id="M68" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M69" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> are the prior and observation error covariance matrices. The statistical distribution of the posterior estimate of <inline-formula><mml:math id="M70" display="inline"><mml:mi mathvariant="bold-italic">x</mml:mi></mml:math></inline-formula>, given the observation operator, <inline-formula><mml:math id="M71" display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M72" display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="bold-italic">y</mml:mi><mml:mi mathvariant="normal">o</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula>, also follows a Gaussian distribution <inline-formula><mml:math id="M73" display="inline"><mml:mrow><mml:mi>N</mml:mi><mml:mo>(</mml:mo><mml:msup><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mi mathvariant="normal">a</mml:mi></mml:msup><mml:mo>,</mml:mo><mml:mi mathvariant="bold">A</mml:mi><mml:mo>)</mml:mo></mml:mrow></mml:math></inline-formula>, with <inline-formula><mml:math id="M74" display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula> being the mean and <inline-formula><mml:math id="M75" display="inline"><mml:mi mathvariant="bold">A</mml:mi></mml:math></inline-formula> being the error covariance matrix characterizing the posterior uncertainty. The problem is solved by deriving the following:

                <disp-formula specific-use="align" content-type="numbered"><mml:math id="M76" display="block"><mml:mtable displaystyle="true"><mml:mlabeledtr id="Ch1.E1"><mml:mtd><mml:mtext>1</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:mi mathvariant="bold">A</mml:mi><mml:mo>=</mml:mo><mml:msup><mml:mfenced close=")" open="("><mml:mrow><mml:msup><mml:mi mathvariant="bold">B</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>+</mml:mo><mml:msup><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msup><mml:msup><mml:mi mathvariant="bold">R</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mi mathvariant="bold">M</mml:mi></mml:mrow></mml:mfenced><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><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 class="stylechange" displaystyle="true"/></mml:mtd><mml:mtd><mml:mrow><mml:mstyle displaystyle="true" class="stylechange"/><mml:msup><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mi mathvariant="normal">a</mml:mi></mml:msup><mml:mo>=</mml:mo><mml:msup><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mi mathvariant="normal">b</mml:mi></mml:msup><mml:mo>+</mml:mo><mml:msup><mml:mi mathvariant="bold">AM</mml:mi><mml:mi mathvariant="normal">T</mml:mi></mml:msup><mml:msup><mml:mi mathvariant="bold">R</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mfenced open="(" close=")"><mml:mrow><mml:msup><mml:mi mathvariant="bold-italic">y</mml:mi><mml:mi mathvariant="normal">o</mml:mi></mml:msup><mml:mo>-</mml:mo><mml:mi mathvariant="bold">M</mml:mi><mml:msup><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mi mathvariant="normal">b</mml:mi></mml:msup><mml:mo>-</mml:mo><mml:msup><mml:mi mathvariant="bold-italic">y</mml:mi><mml:mi mathvariant="normal">fixed</mml:mi></mml:msup></mml:mrow></mml:mfenced><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mlabeledtr></mml:mtable></mml:math></disp-formula>

            where <inline-formula><mml:math id="M77" display="inline"><mml:msup><mml:mi/><mml:mi mathvariant="normal">T</mml:mi></mml:msup></mml:math></inline-formula> and <inline-formula><mml:math id="M78" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> denote the transpose and inverse of a given matrix.</p>
      <p id="d1e1238">Equation (1) shows that A only depends on prior and observation error
covariance matrices, on the observation operator, and implicitly on the
structure of the observation vector (i.e., on the time, location and
representation of the observations in <inline-formula><mml:math id="M79" display="inline"><mml:mi mathvariant="bold">M</mml:mi></mml:math></inline-formula>), while Eq. (2) shows that <inline-formula><mml:math id="M80" display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mi mathvariant="normal">a</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula> also depends on the actual value of <inline-formula><mml:math id="M81" display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mi mathvariant="normal">b</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M82" display="inline"><mml:mrow><mml:msup><mml:mi mathvariant="bold-italic">y</mml:mi><mml:mi mathvariant="normal">o</mml:mi></mml:msup></mml:mrow></mml:math></inline-formula>. PMIF is an analytical inversion system that solves for Eq. (1) or for an approximation of this equation (when accounting for temporal correlations in <inline-formula><mml:math id="M83" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula>) by building the different matrices involved in this equation.</p>
      <p id="d1e1288">We characterize <inline-formula><mml:math id="M84" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula>, <inline-formula><mml:math id="M85" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M86" display="inline"><mml:mi mathvariant="bold">A</mml:mi></mml:math></inline-formula> by the corresponding standard deviations (<inline-formula><mml:math id="M87" display="inline"><mml:mi mathvariant="italic">σ</mml:mi></mml:math></inline-formula>) of uncertainty in individual control parameters or aggregations of control parameters and by the temporal auto-correlations of the uncertainties (Sect. 2.6). In the following, the “uncertainty reduction” for a given control variable or for an aggregation of control variables (like emission budgets over larger timescales than that of the control vector) refers to the relative difference between its prior and posterior uncertainty: <inline-formula><mml:math id="M88" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>-</mml:mo><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="normal">a</mml:mi></mml:msub><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="normal">b</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>.</p>
      <p id="d1e1341">We use a Gaussian plume model (Sect. 2.4) to simulate the atmospheric
transport at a spatial resolution consistent with that of the <inline-formula><mml:math id="M89" 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>
measurements from the planned <inline-formula><mml:math id="M90" 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> imager and with the highly
heterogeneous distribution of emissions. Compared with complex 3-D
atmospheric transport models, Gaussian plume models have a very low
computational cost, making the global assessment of posterior uncertainty
and uncertainty reduction at the scale of emission clumps from the
assimilation of high-resolution data feasible. However, since a Gaussian
plume model provides a highly simplified approximation of the atmospheric
transport from emission clumps, we need to verify that its use in the PMIF
yields estimates of the uncertainties in the inverted emissions that are
consistent with those that would be based on more complex models. Therefore,
we first compare the results for Paris from PMIF against those acquired
based on a 3-D Eulerian atmospheric transport model by Broquet et al. (2018), the latter also
accounting for uncertainties in diffuse <inline-formula><mml:math id="M91" 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> fluxes. On the one hand,
the signals from these diffuse and natural <inline-formula><mml:math id="M92" 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> fluxes cannot be
modeled effectively by a Gaussian plume model. On the other hand, the
diffuse and natural <inline-formula><mml:math id="M93" 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> fluxes in Paris were shown to have only a weak
impact on the inversion of whole-city <inline-formula><mml:math id="M94" 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> emissions (Staufer et al., 2016).
For this comparison, we use the same simulation of the <inline-formula><mml:math id="M95" 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> sampling by
CarbonSat (Sect. 2.2) and a similar control vector to Broquet et al. (2018). The corresponding
inversion with the PMIF is called PMIF-Paris hereafter. Then we apply the
system to all the emission clumps over the globe and over 1 year using a
different control vector and a simulation of the <inline-formula><mml:math id="M96" 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> sampling by a
single CO2M satellite (Sect. 2.2). The inversions for all emission clumps
over the globe are called PMIF-Globe. In PMIF-Globe, we first investigate
the potential of satellite observations in constraining emissions from
individual time windows (ExpNoCor in Sect. 2.6). Then we assess the ability
of satellite observations to constrain emissions at annual scale by
accounting for the temporal auto-correlation of the prior uncertainties
(other experiments in Sect. 2.6). Tables 1 and 2 summarize the different
options for the configuration of the system and of the OSSEs. One
distinction between PMIF-Paris and PMIF-Globe is that PMIF-Paris relates
<inline-formula><mml:math id="M97" 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> signals with the mean emissions 6 h before overpasses, while
it is assumed that in PMIF-Globe that the <inline-formula><mml:math id="M98" 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> signals only provide
effective constraints on 3 h mean emissions before individual overpasses.
The 6 h period corresponds to the period of emissions from Paris whose
signature in the <inline-formula><mml:math id="M99" 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> field can still be detected by the satellite
despite the atmospheric diffusion (Broquet et al., 2018). While Broquet et al. (2018) indicated that the period of “detectable” emissions from a large megacity like Paris could last up to 6 h, most of the clumps across the globe have smaller emission rates than Paris or are located in more complex environment close to other major emission areas where <inline-formula><mml:math id="M100" 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> signals can be attributed to multiple sources, making the detection of the <inline-formula><mml:math id="M101" 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> signature of emissions a few<?pagebreak page5817?> hours before the satellite overpass even more difficult. For the PMIF-Globe experiments, we thus conservatively assume that the <inline-formula><mml:math id="M102" 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> signals can only provide effective constraints on 3 h mean emissions before individual overpasses in general.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><?xmltex \currentcnt{1}?><label>Table 1</label><caption><p id="d1e1504">The configuration of the PMIF-Paris inversion.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="2">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Type of setting</oasis:entry>
         <oasis:entry colname="col2">Option</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Control vector</oasis:entry>
         <oasis:entry colname="col2">6 h mean <inline-formula><mml:math id="M103" 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> emissions from Paris over 05:00–11:00 (local time is used)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Plume length in the computation of <inline-formula><mml:math id="M104" display="inline"><mml:mi mathvariant="bold">M</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">6 h <inline-formula><mml:math id="M105" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> wind speed averaged over 05:00–11:00</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Observation sampling and measurement error</oasis:entry>
         <oasis:entry colname="col2">Simulation of the sampling and random measurement  noise for CarbonSat near Paris</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Prior uncertainty</oasis:entry>
         <oasis:entry colname="col2">22.4 % for the 6 h mean emissions. The potential correlations between the 6 h mean</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">emissions of different days are ignored for the diagnostics</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T2" specific-use="star"><?xmltex \currentcnt{2}?><label>Table 2</label><caption><p id="d1e1602">The different options for the configuration of PMIF-Globe inversions.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="2">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Type of setting</oasis:entry>
         <oasis:entry colname="col2">Option</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Control vector</oasis:entry>
         <oasis:entry colname="col2">For each clump of the globe, 3 h mean emissions over 08:30–11:30 and the mean emissions</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">for the remaining 21 h (00:00–08:30 plus 11:30–24:00) within each day of 1 year</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Plume length in the computation</oasis:entry>
         <oasis:entry colname="col2">3 h <inline-formula><mml:math id="M106" display="inline"><mml:mo>×</mml:mo></mml:math></inline-formula> wind speed averaged over 08:30–11:30; no computation of plume</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">computation of <inline-formula><mml:math id="M107" display="inline"><mml:mi mathvariant="bold">M</mml:mi></mml:math></inline-formula></oasis:entry>
         <oasis:entry colname="col2">for the emissions over 00:00–08:30 plus 11:30–24:00</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Observation sampling and</oasis:entry>
         <oasis:entry colname="col2">Simulation of the sampling and random measurement noise for a single CO2M <inline-formula><mml:math id="M108" 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> imager</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">measurement error</oasis:entry>
         <oasis:entry colname="col2">all over the globe</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Constraint on the prior</oasis:entry>
         <oasis:entry colname="col2">For each clump, the budget of the prior uncertainty in annual emission is 30 %. The uncertainty</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">uncertainty</oasis:entry>
         <oasis:entry colname="col2">in the 3 h mean emissions and in the budget of the emissions for the rest of the day are</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">downscaled depending on the assumptions on the components of the prior  uncertainty</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">and on their temporal auto-correlations (see Sect. 2.6)</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap>

</sec>
<sec id="Ch1.S2.SS2">
  <label>2.2</label><title>Observation space</title>
      <p id="d1e1749">In this study, we consider the samplings from two different virtual <inline-formula><mml:math id="M109" 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>
imagers.</p>
      <p id="d1e1763">The first sampling used in PMIF-Paris (Table 1 and Sect. 2.7.1) is the
simulation of the sampling for CarbonSat by Buchwitz et al. (2013)
exactly as in Broquet et al. (2018). <inline-formula><mml:math id="M110" 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> is sampled by a 240 km swath instrument with 2 km spatial resolution. Given the presence of cloud and aerosol and their impacts on the precision of <inline-formula><mml:math id="M111" 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> retrievals, only “good” <inline-formula><mml:math id="M112" 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> observations, for which the sum of the retrieved aerosol optical depth (AOD) at near-infrared (NIR) wavelength and atmosphere cirrus optical depth (COD) is less than 0.3, are used in the inversions. The preferable condition, <inline-formula><mml:math id="M113" display="inline"><mml:mrow><mml:mtext>AOD(NIR)</mml:mtext><mml:mo>+</mml:mo><mml:mtext>COD</mml:mtext><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.3</mml:mn></mml:mrow></mml:math></inline-formula>, for a good <inline-formula><mml:math id="M114" 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>
observation is referred to as “clear sky” hereafter. The CarbonSat
sampling was simulated over the whole globe and for a full year by Buchwitz
et al. (2013), but it is used here for the inversion of the emission of Paris only. Thus, only the passes with at least one good <inline-formula><mml:math id="M115" 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> measurement in the 100 km radius circle centered on Paris are used, as in Broquet et al. (2018).</p>
      <p id="d1e1838">The second sampling is global and is used for all the other experiments of
PMIF-Globe (Table 2 and Sect. 2.7.2). It corresponds to that of a single
CO2M satellite with a 300 km swath and 2 km spatial resolution. CO2M is
similar to CarbonSat for sampling but has a larger swath and better
precision (Sect. 2.5). The simulation is based on the method and model
described by Buchwitz et al. (2013) but uses different values for the parameters in the model.</p>
</sec>
<sec id="Ch1.S2.SS3">
  <label>2.3</label><title>Control vector</title>
      <p id="d1e1849">In the PMIF-Paris inversion, the satellite observations are sampled at 11:00
local time, in line with the experiments from Broquet et al. (2018). The inversion solves for the mean emissions for the 6 h before 11:00 local time. Broquet et al. (2018) solved for the hourly emissions during this 6 h period but PMIF can only solve for the mean emissions during the 6 h period due to the fact that the Gaussian plume model cannot be used to compute the signatures in the <inline-formula><mml:math id="M116" 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> field of individual hourly emissions during that period. The control vector in PMIF-Paris thus consists of a set of scaling factors for the mean emission between 05:00 and 11:00 for all individual overpasses near Paris (Sect. 2.7.1). The prior and posterior scaling factors are used to rescale the 1 h and <inline-formula><mml:math id="M117" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> km resolution emission fields from an emission map and its temporal profile which are parts of the observation operator (Sect. 2.4).</p>
      <p id="d1e1873">In the PMIF-Globe inversion, the satellite observations are sampled at a
local time of approximately 11:30 over all the clumps. The inversion solves
for a scaling factor for 3 h mean emissions between 08:30 and 11:30 and a
scaling factor for the emissions during of the rest of the day (00:00–08:30
plus 11:30–24:00) for each day over 1 year and for all the clumps over the
globe:
            <disp-formula id="Ch1.E3" content-type="numbered"><label>3</label><mml:math id="M118" display="block"><mml:mtable class="split" rowspacing="0.2ex" columnspacing="1em" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mo>=</mml:mo><mml:mo mathsize="1.5em">[</mml:mo><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mrow><mml:mi mathvariant="normal">clump</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="normal">morning</mml:mi></mml:mrow></mml:msubsup><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mrow><mml:mi mathvariant="normal">clump</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">rest</mml:mi></mml:mrow></mml:msubsup><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mrow><mml:mi mathvariant="normal">clump</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">2</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">morning</mml:mi></mml:mrow></mml:msubsup><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mrow><mml:mi mathvariant="normal">clump</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">2</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">rest</mml:mi></mml:mrow></mml:msubsup><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><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:mi mathvariant="normal">…</mml:mi><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mrow><mml:mi mathvariant="normal">clump</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">366</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">morning</mml:mi></mml:mrow></mml:msubsup><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mrow><mml:mi mathvariant="normal">clump</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">366</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">rest</mml:mi></mml:mrow></mml:msubsup><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mrow><mml:mi mathvariant="normal">clump</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi mathvariant="normal">morning</mml:mi></mml:mrow></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:mspace width="0.25em" linebreak="nobreak"/><mml:mspace linebreak="nobreak" width="0.25em"/><mml:mspace width="0.25em" linebreak="nobreak"/><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mrow><mml:mi mathvariant="normal">clump</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">rest</mml:mi></mml:mrow></mml:msubsup><mml:mo>,</mml:mo><mml:mi mathvariant="normal">…</mml:mi><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mi mathvariant="normal">clumpN</mml:mi><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">366</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">morning</mml:mi></mml:mrow></mml:msubsup><mml:mo>,</mml:mo><mml:msubsup><mml:mi mathvariant="italic">λ</mml:mi><mml:mi mathvariant="normal">clumpN</mml:mi><mml:mrow><mml:mi mathvariant="normal">day</mml:mi><mml:mn mathvariant="normal">366</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="normal">rest</mml:mi></mml:mrow></mml:msubsup><mml:mo mathsize="1.5em">]</mml:mo><mml:mo>.</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula></p>
      <p id="d1e2113">In both types of experiments, we do not include the diffuse emissions
outside the selected clumps and the natural fluxes (more generally, any
parameter of the “background concentrations”, Kuhlmann et al., 2019) in
the control vector. The setup of the <inline-formula><mml:math id="M119" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> matrix also ignores uncertainties in the background concentrations (Sect. 2.5). This is another divergence from the inversion configuration of Broquet et al. (2018), who accounted for such uncertainties.</p>
</sec>
<sec id="Ch1.S2.SS4">
  <label>2.4</label><title>Observation operator</title>
      <?pagebreak page5818?><p id="d1e2131">The observation operator in PMIF (which is used in Eq. 1) is composed of two
sub-operators. The first operator (<inline-formula><mml:math id="M120" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">inventory</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) describes the spatial distribution (within the clumps) and temporal variations of the emissions whose budgets are controlled by the inversion during 08:30–11:30 and during the remaining 21 h for each clump: <inline-formula><mml:math id="M121" display="inline"><mml:mrow><mml:mi mathvariant="bold-italic">x</mml:mi><mml:mo>→</mml:mo><mml:mi mathvariant="bold-italic">E</mml:mi><mml:mo>=</mml:mo><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">inventory</mml:mi></mml:msub><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi mathvariant="bold-italic">x</mml:mi></mml:mrow></mml:math></inline-formula>. The spatial distribution of the emissions are based on estimates from ODIAC (Oda et al., 2018) for the year 2016. ODIAC provides the monthly mean emissions for 12 months through a year at a <inline-formula><mml:math id="M122" display="inline"><mml:mrow><mml:mn mathvariant="normal">0.0083</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">0.0083</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> (approximately <inline-formula><mml:math id="M123" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow><mml:mo>×</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mrow class="unit"><mml:mi mathvariant="normal">km</mml:mi></mml:mrow></mml:mrow></mml:math></inline-formula>) spatial resolution. The weekly and diurnal (at hourly resolution) profiles from the Temporal Improvements for Modeling Emissions by Scaling (TIMES) product (Nassar et al., 2013) are applied to the monthly emission maps of ODIAC to generate the hourly emission fields. The second operator (<inline-formula><mml:math id="M124" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">plume</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) simulates the plumes of <inline-formula><mml:math id="M125" 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> enhancement above the background at and downwind of the emission clumps at 11:30: <inline-formula><mml:math id="M126" display="inline"><mml:mrow><mml:mi mathvariant="bold-italic">E</mml:mi><mml:mo>→</mml:mo><mml:mi mathvariant="bold-italic">y</mml:mi><mml:mo>=</mml:mo><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">plume</mml:mi></mml:msub><mml:mi mathvariant="bold-italic">E</mml:mi></mml:mrow></mml:math></inline-formula>. We assume that the plume of <inline-formula><mml:math id="M127" 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> enhancement related to a given emitting pixel within a clump of the ODIAC map has a Gaussian shape and the plume from a clump is a sum of multiple Gaussian plumes from all the ODIAC pixels within that clump. For a given emitting pixel, the Gaussian plume model writes the following:
            <disp-formula id="Ch1.E4" content-type="numbered"><label>4</label><mml:math id="M128" display="block"><mml:mrow><mml:mi mathvariant="bold-italic">y</mml:mi><mml:mfenced open="(" close=")"><mml:mrow><mml:mi>i</mml:mi><mml:mo>,</mml:mo><mml:mi>j</mml:mi></mml:mrow></mml:mfenced><mml:mo>=</mml:mo><mml:mi mathvariant="italic">α</mml:mi><mml:mstyle displaystyle="true"><mml:mfrac style="display"><mml:mi>E</mml:mi><mml:mrow><mml:msqrt><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mi mathvariant="italic">π</mml:mi></mml:mrow></mml:msqrt><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>j</mml:mi></mml:msub><mml:mi>u</mml:mi></mml:mrow></mml:mfrac></mml:mstyle><mml:msup><mml:mi>e</mml:mi><mml:mrow><mml:mo>-</mml:mo><mml:mstyle scriptlevel="+1"><mml:mfrac><mml:mrow><mml:msup><mml:mi>j</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:mrow><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>j</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mfrac></mml:mstyle></mml:mrow></mml:msup><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
          where <inline-formula><mml:math id="M129" display="inline"><mml:mi mathvariant="bold-italic">y</mml:mi></mml:math></inline-formula> is the <inline-formula><mml:math id="M130" 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> enhancement (in ppm) downwind of the emitting pixel. The <inline-formula><mml:math id="M131" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> direction is parallel to the wind direction, and the <inline-formula><mml:math id="M132" display="inline"><mml:mi>j</mml:mi></mml:math></inline-formula> direction is perpendicular to the wind direction. <inline-formula><mml:math id="M133" display="inline"><mml:mi mathvariant="bold-italic">y</mml:mi></mml:math></inline-formula> depends on the mean emission rate
during 08:30–11:30 at local time (<inline-formula><mml:math id="M134" display="inline"><mml:mi>E</mml:mi></mml:math></inline-formula>, in g s<inline-formula><mml:math id="M135" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>), the wind speed (<inline-formula><mml:math id="M136" display="inline"><mml:mi>u</mml:mi></mml:math></inline-formula>, in m s<inline-formula><mml:math id="M137" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>), the cross-wind distance (<inline-formula><mml:math id="M138" display="inline"><mml:mi>j</mml:mi></mml:math></inline-formula>) and the parameter <inline-formula><mml:math id="M139" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>j</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (see below). The wind direction and speed is taken from the Cross-Calibrated Multi-Platform (CCMP) gridded surface wind fields for the year 2008 (Atlas et al., 2011). The CCMP product uses a variational analysis method (VAM) to combine the data from Version-7 RSS radiometer wind speeds, QuikSCAT and ASCAT scatterometer wind vectors, moored buoy wind data, and ERA-Interim model wind fields. The <inline-formula><mml:math id="M140" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>j</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is a function of downwind distance <inline-formula><mml:math id="M141" display="inline"><mml:mi>i</mml:mi></mml:math></inline-formula> and atmospheric stability parameter <inline-formula><mml:math id="M142" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>j</mml:mi></mml:msub><mml:mo>=</mml:mo><mml:mi mathvariant="italic">β</mml:mi><mml:mi>j</mml:mi><mml:mo>/</mml:mo><mml:mo>(</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>+</mml:mo><mml:mi mathvariant="italic">γ</mml:mi><mml:mi>j</mml:mi><mml:msup><mml:mo>)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>/</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:mrow></mml:math></inline-formula>, where <inline-formula><mml:math id="M143" display="inline"><mml:mi mathvariant="italic">α</mml:mi></mml:math></inline-formula> is a coefficient that converts the computed
<inline-formula><mml:math id="M144" 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> enhancement in the unit of parts per million, and <inline-formula><mml:math id="M145" display="inline"><mml:mi mathvariant="italic">β</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M146" display="inline"><mml:mi mathvariant="italic">γ</mml:mi></mml:math></inline-formula> are
coefficients depending on the atmospheric Pasquill stability category, which
is a function of the wind speed and solar radiation (Turner, 1970). The values for <inline-formula><mml:math id="M147" display="inline"><mml:mi mathvariant="italic">β</mml:mi></mml:math></inline-formula> and <inline-formula><mml:math id="M148" display="inline"><mml:mi mathvariant="italic">γ</mml:mi></mml:math></inline-formula> can be found in Bowers et al. (1980). The original Gaussian plume model generates a stationary plume of an infinite length and width downwind of the emissions. Because we assume that the <inline-formula><mml:math id="M149" 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> plumes sampled from a satellite overpass is only related to the emissions 3 h before, the Gaussian plume corresponding to each emitting pixel is cut off at the downwind distance equaling the wind speed multiplied by 3 h. The width of the plume is also cut off beyond 3 times the value of <inline-formula><mml:math id="M150" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">σ</mml:mi><mml:mi>j</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> in the cross-wind direction. The observation operator is null for emission of the remaining 21 h (00:00–08:30 plus 11:30–24:00).</p>
      <p id="d1e2552">The size of the full theoretical control vector corresponds to 11 314
emission clumps times 2 time windows for each day times 366 d. The size
of this full theoretical observation vector over the year is thus more than
30 000 000. Building matrices and applying Eq. (1) with such spaces is, in
practice, not computationally affordable. Therefore, we divide the globe
into 5400 spatial inversion windows (from 180<inline-formula><mml:math id="M151" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> W to
180<inline-formula><mml:math id="M152" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> E and from 90<inline-formula><mml:math id="M153" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> N to 60<inline-formula><mml:math id="M154" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> S), each inversion window covering an area of <inline-formula><mml:math id="M155" display="inline"><mml:mrow><mml:mn mathvariant="normal">10</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">10</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> and being extended on the four boundaries with margins of 500 km to ensure that the plumes from the clumps near the boundary of inversion windows are fully simulated and accounted for in the corresponding inversions. <inline-formula><mml:math id="M156" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">plume</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> is constructed with a set of block matrices, each block representing a single spatial inversion window and a single day. When an emission clump and its plume are comprised within more than one inversion window on a single day, only the results obtained in the window that covers the full plume is used in <inline-formula><mml:math id="M157" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">plume</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>.</p>
</sec>
<sec id="Ch1.S2.SS5">
  <label>2.5</label><title>Observation error</title>
      <p id="d1e2643">We evaluate the projection of the measurement noise of the satellite
observation and ignore uncertainties in the observation operator. The
measurement noise is derived from the<?pagebreak page5819?> simulations of random measurement
errors from Buchwitz et al. (2013), and the impact of the systematic measurement errors is ignored. The random measurement errors are simulated as a function of geographic location (e.g., solar zenith angle, SZA), surface (e.g., albedo) and atmosphere characteristics (e.g., AOD). The random measurement error is 1.4 ppm for vegetation albedo and SZA 50<inline-formula><mml:math id="M158" display="inline"><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:math></inline-formula> in the CS sampling, and it is 0.7 ppm in the CO2M sampling, thus being 2 times smaller for the latter. The random measurement errors are uncorrelated from one <inline-formula><mml:math id="M159" 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> data to the other, and the <inline-formula><mml:math id="M160" display="inline"><mml:mi mathvariant="bold">R</mml:mi></mml:math></inline-formula> matrix is thus a diagonal matrix as generally done in atmospheric inversion.</p>
</sec>
<sec id="Ch1.S2.SS6">
  <label>2.6</label><title>Specification of the prior uncertainties and of their temporal
auto-correlations</title>
      <p id="d1e2681">Two configurations for the prior uncertainty are used in the OSSEs (Sect. 2.7). In the PMIF-Paris inversion, the prior uncertainty is 22.4 % for the each of the scaling factors for 6 h mean emission, the choice of this
value being consistent with the configuration used by Broquet et al. (2018).</p>
      <p id="d1e2684">In the PMIF-Globe inversions, the prior uncertainty is downscaled from its
estimate for the annual budget of emissions of each clump. A prior
uncertainty in annual emission of 30 % is assumed for all clumps. This
value is chosen to be of the same order of magnitude as the typical
difference between emission inventories for a single point source and city.
For example, Gurney et al. (2016) found that one-fifth of the power plants had monthly emission differences larger than 13 % between the estimates by two different US agencies. Gurney et al. (2019) compared the emission maps from ODIAC and Hestia for four US cities and found the whole-city differences are between <inline-formula><mml:math id="M161" display="inline"><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1.5</mml:mn></mml:mrow></mml:math></inline-formula> % and <inline-formula><mml:math id="M162" display="inline"><mml:mrow><mml:mo>+</mml:mo><mml:mn mathvariant="normal">20.8</mml:mn></mml:mrow></mml:math></inline-formula> %. Gately and Hutyra (2017) compared the inventories reported by local authorities and bottom-up fossil fuel <inline-formula><mml:math id="M163" 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> emission maps for 11 US cities and found the differences range from 33 % to 78 %. Then, the downscaling of the uncertainty in annual emissions into uncertainties at the sub-daily scale of the control variables (i.e., 3 h mean emission over 08:30–11:30 and 21 h mean emission during the rest of the day; Sect. 2.3) follows a decomposition of the total uncertainty into components with different temporal auto-correlations.</p>
      <p id="d1e2718">The hourly emissions in inventories are usually derived from the periodic
typical temporal profiles to annual emissions (Andres et al., 2011; Nassar et al., 2013). There are large variations in actual emissions from hour to hour and from day to day, resulting in large differences between the emission
estimates derived based on typical temporal profiles and actual emissions.
These differences are sources of uncertainties in the emission inventories
which are used in the inversion as prior information. However, there is no
consensus regarding the uncertainty in emission inventories and their error
structures (Gurney et al., 2019). We compare the typical temporal profiles of transport emissions and energy sector from the TIMES product with the TOMTOM traffic index (<uri>https://www.tomtom.com/en_gb/</uri>, last access: 20 September 2020, which provides indications of the level of variability in the traffic, though not of that of the <inline-formula><mml:math id="M164" 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> emissions themselves), respectively, and with the actual hourly <inline-formula><mml:math id="M165" 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> emissions from electricity production in France (<uri>https://www.services-rte.com/en/home.html</uri>, last access: 17 July 2017). Although these comparisons are only made for two sectors, the results already show that it is challenging
to describe the temporal auto-correlations of the uncertainty in emissions
with simple exponentially decaying functions (Figs. S1 and S2 in the Supplement) like what is usually done in traditional atmospheric inversions (Chevallier et al., 2010; Kountouris et al., 2015). We thus make several assumptions regarding the decomposition of the prior uncertainty into components with different modes of auto-correlation.</p>
      <p id="d1e2749">In some scenarios, we consider an “annual component” that is fully
correlated in time over 1 year. We also consider “uncorrelated” components
whose temporal auto-correlations are null and “sub-annual” components
whose temporal auto-correlations follow the exponential decaying model with
a correlation length smaller than 1 year. Specifically, we assume that the
correlation between two instants of the sub-annual component at hourly scale
is described by the following:
            <disp-formula id="Ch1.E5" content-type="numbered"><label>5</label><mml:math id="M166" display="block"><mml:mrow><mml:mi>r</mml:mi><mml:mo>=</mml:mo><mml:mi>exp⁡</mml:mi><mml:mfenced open="(" close=")"><mml:mrow><mml:mo>-</mml:mo><mml:mi mathvariant="normal">Δ</mml:mi><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>h</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:mfenced><mml:mo>×</mml:mo><mml:mi>exp⁡</mml:mi><mml:mfenced close=")" open="("><mml:mrow><mml:mo>-</mml:mo><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi>d</mml:mi><mml:mo>/</mml:mo><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:mfenced><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
          where <inline-formula><mml:math id="M167" display="inline"><mml:mrow><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi>h</mml:mi></mml:mrow></mml:math></inline-formula> is the time lag (in hours) between the two times of the day
that are considered, and <inline-formula><mml:math id="M168" display="inline"><mml:mrow><mml:mi mathvariant="normal">Δ</mml:mi><mml:mi>d</mml:mi></mml:mrow></mml:math></inline-formula> is the time lag (in days) between the two
dates that are considered. The parameters <inline-formula><mml:math id="M169" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M170" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> follow the fit of the misfits between the TIMES profiles and the TOMTOM and electricity production indices to the exponential functions at
the hourly scale and at the daily scale, respectively (Figs. S1 and S2). The temporal
auto-correlations between the emissions during the aggregated time windows
(08:30–11:30 and the remaining 21 h) are computed by re-aggregating the
uncertainties at the hourly scale, accounting for temporal auto-correlation.</p>
      <p id="d1e2844">The detailed configuration of the different scenarios for the decomposition
of the prior uncertainty are listed below:
<list list-type="custom"><list-item><label>1.</label>
      <p id="d1e2849"><italic>Annual component and moderately correlated sub-annual component (AMS).</italic> This is composed of an annual component and a sub-annual component. The temporal auto-correlation of the sub-annual component follows Eq. (5) with <inline-formula><mml:math id="M171" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:math></inline-formula> h and <inline-formula><mml:math id="M172" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">7</mml:mn></mml:mrow></mml:math></inline-formula> d. The ratio of the uncertainty in the annual component to that in the sub-annual component for 3 h emissions is assumed to be <inline-formula><mml:math id="M173" display="inline"><mml:mrow><mml:mn mathvariant="normal">3</mml:mn><mml:mo>:</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula>. This leads to an annual uncertainty component <inline-formula><mml:math id="M174" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 29 %) and a sub-annual component <inline-formula><mml:math id="M175" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 49 %) for 3 h emissions and <inline-formula><mml:math id="M176" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 38 %) for 21 h emissions.</p></list-item><list-item><label>2.</label>
      <p id="d1e2928"><italic>Annual component and strongly correlated sub-annual component (ASS).</italic> This is composed of an annual component and a sub-annual component. The temporal<?pagebreak page5820?> auto-correlation of the sub-annual component follows Eq. (5) with <inline-formula><mml:math id="M177" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2400</mml:mn></mml:mrow></mml:math></inline-formula> h, which approximately corresponds to having full correlations between hourly uncertainties within a single day, and <inline-formula><mml:math id="M178" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">20</mml:mn></mml:mrow></mml:math></inline-formula> d. The ratio of the uncertainty in the annual component to that in the sub-annual component for 3 h emissions is assumed to be <inline-formula><mml:math id="M179" display="inline"><mml:mrow><mml:mn mathvariant="normal">3</mml:mn><mml:mo>:</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula>. This leads to an annual uncertainty component <inline-formula><mml:math id="M180" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 26 %) and a sub-annual component <inline-formula><mml:math id="M181" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 44 %) for 3 h emissions and <inline-formula><mml:math id="M182" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 44 %) for 21 h emissions.</p></list-item><list-item><label>3.</label>
      <p id="d1e3007"><italic>Moderately correlated sub-annual component (MCS).</italic> This is composed of a sub-annual component. The temporal auto-correlation of the sub-annual component follows Eq. (5) with <inline-formula><mml:math id="M183" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:math></inline-formula> h and <inline-formula><mml:math id="M184" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">7</mml:mn></mml:mrow></mml:math></inline-formula> d. This leads to a sub-annual component <inline-formula><mml:math id="M185" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 198 %) for 3 h emissions and <inline-formula><mml:math id="M186" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 119 %) for 21 h emissions.</p></list-item><list-item><label>4.</label>
      <p id="d1e3063"><italic>Strongly correlated sub-annual component (SCS).</italic> This is composed of a sub-annual component. The temporal auto-correlation of the sub-annual component follows Eq. (5) with <inline-formula><mml:math id="M187" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2400</mml:mn></mml:mrow></mml:math></inline-formula> h and <inline-formula><mml:math id="M188" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">20</mml:mn></mml:mrow></mml:math></inline-formula> d. This leads to a sub-annual component <inline-formula><mml:math id="M189" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 93 %) for 3 h emissions and <inline-formula><mml:math id="M190" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 93 %) for 21 h emissions.</p></list-item><list-item><label>5.</label>
      <p id="d1e3119"><italic>Sector-dependent correlated sub-annual component (SectCS).</italic> This is composed of a sub-annual component for each emission sector. It is assumed that the relative uncertainty for different sectors are the same. The temporal auto-correlation of the sub-annual components for all sectors follow the same formulation as in Eq. (5), but with different <inline-formula><mml:math id="M191" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> and <inline-formula><mml:math id="M192" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula>. For the emissions in the industry sector, <inline-formula><mml:math id="M193" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2400</mml:mn></mml:mrow></mml:math></inline-formula> h and <inline-formula><mml:math id="M194" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">180</mml:mn></mml:mrow></mml:math></inline-formula> d; for the emissions in the transport sector, <inline-formula><mml:math id="M195" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">12</mml:mn></mml:mrow></mml:math></inline-formula> h and <inline-formula><mml:math id="M196" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">7</mml:mn></mml:mrow></mml:math></inline-formula> d; for the emissions from energy sector, <inline-formula><mml:math id="M197" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">24</mml:mn></mml:mrow></mml:math></inline-formula> h and <inline-formula><mml:math id="M198" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">7</mml:mn></mml:mrow></mml:math></inline-formula> d; and for the emissions from other sectors, <inline-formula><mml:math id="M199" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">24</mml:mn></mml:mrow></mml:math></inline-formula> h and <inline-formula><mml:math id="M200" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">14</mml:mn></mml:mrow></mml:math></inline-formula> d. For each clump, the share of emissions from each sector are estimated according to EDGARv4.3.2 (<uri>https://edgar.jrc.ec.europa.eu/</uri>, last access: 25 July 2019). This leads to an uncertainty in 3 h emissions ranges between 40 % and 198 %, and in 21 h emissions ranges between 40 % and 154 %.</p></list-item><list-item><label>6.</label>
      <p id="d1e3271"><italic>No temporal auto-correlation (NoCor).</italic> We assume that the uncertainties in 3 h emissions and 21 h emissions on all days are all random and uncorrelated from one time window to the other, or from one day to the other. The resulting sub-annual component follows the distribution <inline-formula><mml:math id="M201" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 1623 %) for 3 h emissions and <inline-formula><mml:math id="M202" display="inline"><mml:mrow><mml:mo>∼</mml:mo><mml:mi>N</mml:mi></mml:mrow></mml:math></inline-formula>(0, 614 %) for 21 h emissions.</p></list-item></list></p>
      <p id="d1e3296">The prior uncertainty in the 3 h mean emissions between 08:30 and 11:30 is
close to or larger than 100 % in scenarios SCS and MCS, and it even reaches an abnormally huge value of 1623 % in NoCor. Andres et al. (2016) estimated the uncertainty in the widely used emission map CDIAC (Carbon Dioxide Information Analysis Center). They found that the average uncertainty in monthly emissions for one <inline-formula><mml:math id="M203" display="inline"><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> grid cell is 120 % and further suspected that the uncertainties in hourly and daily emissions at urban scale could be even larger (from a few percent to 1000 %). But these large values challenge the assumption that the uncertainty in anthropogenic emissions is normally distributed (Gurney et al., 2019). In this study, we follow the traditional assumption used in atmospheric inversions that the prior uncertainty follows a Gaussian distribution, allowing the prior uncertainty to exceed 100 % in some scenarios. This assumption ensures that the system is analytically solvable using Eqs. (1) and (2). In addition, we focus our analysis on 08:30–11:30 time windows or days for which the posterior uncertainties of underlying emissions are smaller than 20 % (Sect. 2.7.2), a value that is significantly smaller than the prior uncertainty in any scenario. In these cases, Eq. (1) ensures that the posterior uncertainty is almost driven by the projection of the observation error on the control space and is not sensitive to the level of prior uncertainty.</p>
</sec>
<sec id="Ch1.S2.SS7">
  <label>2.7</label><title>Practical implementation of the OSSEs</title>
      <p id="d1e3327">Two sets of OSSEs are conducted under different configurations adapted to
different purposes, as described below. Tables 1 and 2 summarize the
different configurations of the OSSEs.</p>
<sec id="Ch1.S2.SS7.SSS1">
  <label>2.7.1</label><title>Comparison of results between PMIF and a previous study on a single city: Paris</title>
      <p id="d1e3337">In the first OSSE PMIF-Paris, the configuration of the control vector,
observation sampling and errors, and prior uncertainties are made such that
they resemble those in the MC-2 experiments from Broquet et al. (2018): (1) the inversion controls the 6 h mean emissions from Paris before the satellite overpasses on single days; (2) the observation sampling and errors are obtained from CarbonSat mission simulation (Buchwitz et al., 2013). We ignore temporal auto-correlation of the uncertainty in scaling factors for 6 h mean emissions between different days. We select the same 69 satellite CarbonSat overpasses over Paris during 1 year as Broquet et al. (2018). The 31 d of
October 2010 are used to provide a wide sample of atmospheric transport
conditions, i.e., 31 wind fields. These atmospheric transport conditions are
combined with the 69 sets of CarbonSat overpasses (with various cloud and
aerosol coverage) to form 2139 inversion samples. The results for different
overpasses using the same wind field of a single day are ranked according to
the uncertainty reductions and are compared to those obtained in Broquet et
al. (2018).</p>
</sec>
<sec id="Ch1.S2.SS7.SSS2">
  <label>2.7.2</label><title>Applying the PMIF over all emission clumps across the globe</title>
      <p id="d1e3348">In this second set of OSSEs, PMIF-Globe, we conduct inversions for all the
clumps over 1 year. However, the large<?pagebreak page5821?> sizes of the control vector, of the
observation vector and of the associated covariance matrices prevent the
derivation of a full A for all the clumps and all the time windows using Eq. (1). In PMIF, we thus propose and apply a two-step computation that
approximates Eq. (1). This computation assumes that the system has a limited
capability to improve the separation between plumes from distinct clumps on
a given day by crossing the information obtained from different days. In
that sense, the inversion considers the uncertainty reduction obtained for
individual days when considering all the clumps together (first step, see
below) before focusing on individual clumps to account for temporal
correlations in the prior uncertainty (the second step, see below). In other
words, we assume that when crossing information between different time
windows for a given clump, the impact of filtering information from
different spatial overlaps of plumes on different days is relatively smaller
than that of temporal auto-correlation in the prior uncertainty. It is shown
that this method provides a good approximation of <inline-formula><mml:math id="M204" display="inline"><mml:mi mathvariant="bold">A</mml:mi></mml:math></inline-formula> at daily to annual
scales for individual clumps (Sect. S1 in the Supplement).</p>
      <p id="d1e3358">In a first step, Eq. (1) is applied to each <inline-formula><mml:math id="M205" display="inline"><mml:mrow><mml:mn mathvariant="normal">10</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">10</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> spatial inversion window on each day separately (corresponding to an 08:30–11:30 time window for clumps within the spatial inversion windows), by using the corresponding blocks in <inline-formula><mml:math id="M206" display="inline"><mml:mi mathvariant="bold">B</mml:mi></mml:math></inline-formula>:
              <disp-formula id="Ch1.E6" content-type="numbered"><label>6</label><mml:math id="M207" display="block"><mml:mrow><mml:msub><mml:mi mathvariant="bold">A</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>p</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>q</mml:mi></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mo mathsize="1.5em">(</mml:mo><mml:msubsup><mml:mi mathvariant="bold">B</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>p</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>q</mml:mi></mml:mrow><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msubsup><mml:mo>+</mml:mo><mml:msubsup><mml:mi mathvariant="bold">M</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>p</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>q</mml:mi></mml:mrow><mml:mi mathvariant="normal">T</mml:mi></mml:msubsup><mml:msubsup><mml:mi mathvariant="bold">R</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>p</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>q</mml:mi></mml:mrow><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msubsup><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>p</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>q</mml:mi></mml:mrow></mml:msub><mml:msup><mml:mo mathsize="1.5em">)</mml:mo><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
            where <inline-formula><mml:math id="M208" display="inline"><mml:mi>p</mml:mi></mml:math></inline-formula> is the <inline-formula><mml:math id="M209" display="inline"><mml:mi>p</mml:mi></mml:math></inline-formula>th spatial inversion window and <inline-formula><mml:math id="M210" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula> is the <inline-formula><mml:math id="M211" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula>th day during 1 year. Here, <inline-formula><mml:math id="M212" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">B</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>p</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>q</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is a diagonal matrix that only contains the variances of prior uncertainties in emissions during 08:30–11:30 for the clumps within the spatial inversion window. <inline-formula><mml:math id="M213" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>p</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>q</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> accounts for the spatial overlap of plumes generated from nearby clumps. Then we derive an “instant” scalar to represent the observational constraint for a given clump <inline-formula><mml:math id="M214" display="inline"><mml:mi>s</mml:mi></mml:math></inline-formula> in the 08:30–11:30 time window on day <inline-formula><mml:math id="M215" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula> (denoted as <inline-formula><mml:math id="M216" display="inline"><mml:mrow><mml:msub><mml:mi>r</mml:mi><mml:mrow><mml:mi>q</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> hereafter):
              <disp-formula id="Ch1.E7" content-type="numbered"><label>7</label><mml:math id="M217" display="block"><mml:mrow><mml:msub><mml:mi>r</mml:mi><mml:mrow><mml:mi>q</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>s</mml:mi></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>/</mml:mo><mml:msub><mml:mi>a</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>q</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>s</mml:mi></mml:mrow></mml:msub><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn><mml:mo>/</mml:mo><mml:msub><mml:mi>b</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>q</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>s</mml:mi></mml:mrow></mml:msub><mml:mo>,</mml:mo></mml:mrow></mml:math></disp-formula>
            where <inline-formula><mml:math id="M218" display="inline"><mml:mrow><mml:msub><mml:mi>a</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>q</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is a scalar on the diagonal of <inline-formula><mml:math id="M219" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">A</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>p</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>q</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> representing the variance of posterior uncertainty of emission from clump <inline-formula><mml:math id="M220" display="inline"><mml:mi>s</mml:mi></mml:math></inline-formula> in the <inline-formula><mml:math id="M221" display="inline"><mml:mi>p</mml:mi></mml:math></inline-formula>th spatial inversion window and in the 08:30–11:30 time window on day <inline-formula><mml:math id="M222" display="inline"><mml:mi>q</mml:mi></mml:math></inline-formula> obtained by Eq. (2),
and <inline-formula><mml:math id="M223" display="inline"><mml:mrow><mml:msub><mml:mi>b</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mi>q</mml:mi><mml:mo>,</mml:mo><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is a scalar on the diagonal of <inline-formula><mml:math id="M224" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">B</mml:mi><mml:mrow><mml:mi mathvariant="normal">spt</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>p</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>q</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> representing the variance of prior uncertainty for the same control variable.</p>
      <p id="d1e3778">In the second step, the inversion is conducted for each clump <inline-formula><mml:math id="M225" display="inline"><mml:mi>s</mml:mi></mml:math></inline-formula> separately,
considering the correlation in time in the prior uncertainties, using
<inline-formula><mml:math id="M226" display="inline"><mml:mrow><mml:msub><mml:mi>r</mml:mi><mml:mrow><mml:mi>q</mml:mi><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> derived from the first step:
              <disp-formula id="Ch1.E8" content-type="numbered"><label>8</label><mml:math id="M227" display="block"><mml:mtable class="split" rowspacing="0.2ex" columnspacing="1em" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:msub><mml:mi mathvariant="bold">A</mml:mi><mml:mrow><mml:mi mathvariant="normal">tmp</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><?xmltex \hack{\hbox\bgroup\fontsize{9.1}{9.1}\selectfont$\displaystyle}?><mml:mo>=</mml:mo><mml:msup><mml:mfenced open="(" close=")"><mml:mrow><mml:msubsup><mml:mi mathvariant="bold">B</mml:mi><mml:mrow><mml:mi mathvariant="normal">tmp</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>s</mml:mi></mml:mrow><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msubsup><mml:mo>+</mml:mo><mml:mfenced close="]" open="["><mml:mtable class="matrix" columnalign="center center center center center center center" framespacing="0em"><mml:mtr><mml:mtd><mml:mrow><mml:msub><mml:mi>r</mml:mi><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋯</mml:mi></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋯</mml:mi></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mrow><mml:msub><mml:mi>r</mml:mi><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋯</mml:mi></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋯</mml:mi></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mi mathvariant="normal">⋮</mml:mi></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋮</mml:mi></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋮</mml:mi></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋮</mml:mi></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋱</mml:mi></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋮</mml:mi></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋮</mml:mi></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋯</mml:mi></mml:mtd><mml:mtd><mml:mrow><mml:msub><mml:mi>r</mml:mi><mml:mrow><mml:mn mathvariant="normal">366</mml:mn><mml:mo>,</mml:mo><mml:mspace linebreak="nobreak" width="0.125em"/><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mrow><mml:mn mathvariant="normal">0</mml:mn><mml:mi>l</mml:mi><mml:mi>l</mml:mi></mml:mrow></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋯</mml:mi></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd><mml:mtd><mml:mn mathvariant="normal">0</mml:mn></mml:mtd></mml:mtr></mml:mtable></mml:mfenced></mml:mrow></mml:mfenced><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup><mml:mo>,</mml:mo><?xmltex \hack{$\egroup}?></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula>
            where <inline-formula><mml:math id="M228" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">B</mml:mi><mml:mrow><mml:mi mathvariant="normal">tmp</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:math></inline-formula> is the covariance matrix of the prior uncertainty for a given clump <inline-formula><mml:math id="M229" display="inline"><mml:mi>s</mml:mi></mml:math></inline-formula> including the temporal auto-correlation:
              <disp-formula id="Ch1.E9" content-type="numbered"><label>9</label><mml:math id="M230" display="block"><mml:mtable class="split" rowspacing="0.2ex" columnspacing="1em" displaystyle="true" columnalign="right left"><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:msub><mml:mi mathvariant="bold">B</mml:mi><mml:mrow><mml:mi mathvariant="normal">tmp</mml:mi><mml:mo>,</mml:mo><mml:mspace width="0.125em" linebreak="nobreak"/><mml:mi>s</mml:mi></mml:mrow></mml:msub></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd/><mml:mtd><mml:mrow><mml:mo>=</mml:mo><mml:mfenced close="]" open="["><mml:mtable class="matrix" columnalign="center center center center" framespacing="0em"><mml:mtr><mml:mtd><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mtext>cov</mml:mtext><mml:mfenced close=")" open="("><mml:mrow><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msub><mml:mo>,</mml:mo><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:mfenced></mml:mrow></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋯</mml:mi></mml:mtd><mml:mtd><mml:mrow><mml:mtext>cov</mml:mtext><mml:mfenced close=")" open="("><mml:mrow><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msub><mml:mo>,</mml:mo><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mi mathvariant="normal">tn</mml:mi></mml:msub></mml:mrow></mml:mfenced></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mrow><mml:mtext>cov</mml:mtext><mml:mfenced open="(" close=")"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msub><mml:mo>,</mml:mo><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:mfenced></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋯</mml:mi></mml:mtd><mml:mtd><mml:mrow><mml:mtext>cov</mml:mtext><mml:mfenced open="(" close=")"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub><mml:mo>,</mml:mo><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mi mathvariant="normal">tn</mml:mi></mml:msub></mml:mrow></mml:mfenced></mml:mrow></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mi mathvariant="normal">⋮</mml:mi></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋮</mml:mi></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋱</mml:mi></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋮</mml:mi></mml:mtd></mml:mtr><mml:mtr><mml:mtd><mml:mrow><mml:mtext>cov</mml:mtext><mml:mfenced close=")" open="("><mml:mrow><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msub><mml:mo>,</mml:mo><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mi mathvariant="normal">tn</mml:mi></mml:msub></mml:mrow></mml:mfenced></mml:mrow></mml:mtd><mml:mtd><mml:mrow><mml:mtext>cov</mml:mtext><mml:mfenced open="(" close=")"><mml:mrow><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mrow><mml:mi mathvariant="normal">t</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub><mml:mo>,</mml:mo><mml:msub><mml:mi mathvariant="italic">ε</mml:mi><mml:mi mathvariant="normal">tn</mml:mi></mml:msub></mml:mrow></mml:mfenced></mml:mrow></mml:mtd><mml:mtd><mml:mi mathvariant="normal">⋯</mml:mi></mml:mtd><mml:mtd><mml:mrow><mml:msubsup><mml:mi mathvariant="italic">σ</mml:mi><mml:mi mathvariant="normal">tn</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msubsup></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:mfenced><mml:mo>,</mml:mo></mml:mrow></mml:mtd></mml:mtr></mml:mtable></mml:math></disp-formula>
            where <inline-formula><mml:math id="M231" display="inline"><mml:mrow><mml:mi>n</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">366</mml:mn><mml:mo>×</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula>, corresponds to the number of 08:30–11:30 time windows and the rest of the 21 h over the 366 d of 1 year (2008). t1,
t3, etc. represent the 08:30–11:30 time windows and t2, t4, etc. represent
the rest of the 21 h.</p>
      <p id="d1e4315">In PMIF-Globe, we first conduct the inversion in which the prior uncertainty
has no temporal auto-correlation (Exp-NoCor). This is made by applying step 1 to all the <inline-formula><mml:math id="M232" display="inline"><mml:mrow><mml:mn mathvariant="normal">10</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">10</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> spatial inversion windows and all the days separately. This case is used to label the “well constrained” 08:30–11:30 time windows for a given clump when the associated plume is sufficiently well sampled by the <inline-formula><mml:math id="M233" 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> observation to yield a posterior uncertainty in the 3 h mean emission that is smaller than 20 %. We then conduct inversions with different assumptions about the decomposition of the prior uncertainty, accounting for the impact of temporal auto-correlations of the prior uncertainty by applying step 2 of
the inversions. The posterior uncertainties in the 3 h mean emissions
labeled in Exp-NoCor are compared among different inversions to show the
benefit of crossing information from different time windows. Apart from the
assessment of the posterior uncertainties for the 3 h mean emissions, we
also evaluate, for all the experiments except Exp-NoCor, the posterior
uncertainty in daily emissions and in annual emissions by aggregating the
posterior uncertainty covariance matrix <inline-formula><mml:math id="M234" display="inline"><mml:mi mathvariant="bold">A</mml:mi></mml:math></inline-formula> at the corresponding scales obtained in step 2 of the inversions.</p>
</sec>
</sec>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Results</title>
<sec id="Ch1.S3.SS1">
  <label>3.1</label><title>Comparison between results from PMIF and a more complex but local system over an isolated megacity: Paris</title>
      <p id="d1e4373">The comparison of the results from the PMIF-Paris experiment to that of
Broquet et al. (2018) is used to demonstrate that the PMIF produces meaningful statistics for other<?pagebreak page5822?> clumps despite its relative simplicity at the local scale (its complexity being linked to its global and annual coverage). Figure 1 shows the theoretical uncertainty reduction for the 6 h mean emissions obtained in PMIF-Paris inversions with the 1st, 5th, 10th, 15th, 19th and 25th best observation sampling from CarbonSat over 31 inversion days (Sect. 2.7.1), each day being characterized by the average wind speed over Paris. We compare these results with the Fig. 6 from Broquet et al. (2018). Like Broquet et al. (2018), Fig. 1 illustrates the strong correlation between the uncertainty reduction and the average wind speed, indicating that lower wind speed results in a larger signal close to the city that is easier to assimilate than elongated plumes under large wind speeds. For the best observation sampling, the uncertainty reduction remains smaller than 40 % when the wind speed is larger than 13 m s<inline-formula><mml:math id="M235" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, and this value is generally twice as low as the values obtained when the wind speed is smaller than 5 m s<inline-formula><mml:math id="M236" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>.</p>
      <p id="d1e4400">Some differences are seen in Fig. S3, between the results obtained by PMIF
and by Broquet et al. (2018). For example, the PMIF-Paris inversion slightly overestimates the uncertainty reduction under high wind speed (<inline-formula><mml:math id="M237" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">15</mml:mn></mml:mrow></mml:math></inline-formula> m s<inline-formula><mml:math id="M238" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) using the best observation sampling compared to Broquet et al. (2018). These differences reflect the impact of using the Gaussian plume model instead of a 3-D atmospheric transport model, and more importantly, the impact of accounting for more sources of uncertainties (in diffuse emissions and natural fluxes) in Broquet et al. (2018). Despite these differences, the general coherence in the ranges of uncertainty reductions (Fig. S3) under different wind speeds between the PMIF-Paris experiment and Broquet et al. (2018) is a strong indication that the PMIF generates the correct order of magnitude for the uncertainty reduction for a single clump. In addition, Nassar et al. (2017) used the Gaussian plume model to process actual <inline-formula><mml:math id="M239" 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> plumes generated from several power plants, which were sampled by OCO-2, adding the indication that Gaussian plume model can simulate the typical spread and amplitude of actual <inline-formula><mml:math id="M240" 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> plumes and thus support the application of PMIF to a large range of clumps.</p>
      <p id="d1e4447">Figure 1 shows that the uncertainty reduction on 6-hourly emissions from
Paris before the satellite overpass can be up to 74 % under calm wind
conditions (wind speed <inline-formula><mml:math id="M241" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:math></inline-formula> m s<inline-formula><mml:math id="M242" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) with the best observation sampling (in clear sky and with the satellite swath nearly centered on Paris), while it is systematically smaller than 45 % for the 25th best observation sampling, over a full year of CS simulation. In addition, the uncertainty reductions have a large variation for a narrow range of wind speeds, illustrating the strong impacts of the satellite track position with respect to the target and plume, together with the fraction of “clear sky” that modulates the sampling. In particular, the number of observations sampling the plume on the days when the wind direction is perpendicular to
the satellite overpass tends to be lower than the number of days when the wind
direction is parallel to the satellite overpass. This is illustrated in Fig. 1 by the uncertainty reductions on the days when the wind speeds are 1.73, 7.6 and 8.1 m s<inline-formula><mml:math id="M243" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, which are lower than on the days with similar wind speeds.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1"><?xmltex \currentcnt{1}?><label>Figure 1</label><caption><p id="d1e4487">Theoretical uncertainty reduction for the 6 h mean emissions in the
PMIF-Paris experiments using the 1st (red), 5th (orange), 10th (light
green), 15th (purple), 19th (blue) and 25th (green) best observation
sampling from the CarbonSat simulation. The results from the 31 inversion
days are given as a function of the average wind speed over the Paris clump.
A comparison with the results from Broquet et al. (2018) is given in Fig. S3.</p></caption>
          <?xmltex \igopts{width=236.157874pt}?><graphic xlink:href="https://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020-f01.png"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS2">
  <label>3.2</label><?xmltex \opttitle{Potential of space observations for monitoring {$\protect\chem{CO_{2}}$} emissions from individual clumps over 3\,h time windows}?><title>Potential of space observations for monitoring <inline-formula><mml:math id="M244" 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> emissions from individual clumps over 3 h time windows</title>
      <p id="d1e4516">Figure 2a shows the distribution of the number of 08:30–11:30 time windows per
clump for which the posterior uncertainty of 3 h mean emissions is smaller
than 20 % (this number is called N20) in Exp-NoCor. Clumps with small emission budgets tend to have lower N20 values than those with large budgets, due to the fact that the atmospheric plume generated by small
emission clumps is difficult to distinguish from the measurement noise.
Typically, N20 is smaller than 5 d for clumps emitting less than 2 MtC yr<inline-formula><mml:math id="M245" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (like the city of Aswan, Egypt). Conversely, N20 is larger than 10 d for clumps emitting more than 2 MtC yr<inline-formula><mml:math id="M246" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (like the cities of Manchester, UK; Boston, USA; and Chongqing, China). Note that clumps with emissions larger than 2 MtC, although representing less than 25 % of the total number of clumps, contribute more than 83 % of the total clump emissions. At regional scale (Figs. S4, S5), South America, North America, and Africa tend to have larger N20 values for same bin of clump annual emission than the other regions, while the Middle East and Asia have the lowest ones. In addition, there are large variations and spatial heterogeneity in the N20<?pagebreak page5823?> values within each emission bins (Fig. S5), which will be further discussed in Sect. 4.</p>
      <p id="d1e4543">We also show the numbers of 08:30–11:30 time windows per clump being labeled
as “well-constrained” when the posterior uncertainty of 3 h mean emission
is smaller than other thresholds, e.g., 10 % and 30 % (Fig. 2b). In
general, using a posterior uncertainty larger than 20 % as a threshold, we could expect more “well-constrained” cases. But for a given threshold, we still find the number of well-constrained cases increases with the emission budgets.</p>
      <p id="d1e4546">Figure 3 shows the posterior uncertainty in the clump emissions for the
“well constrained” 08:30–11:30 time windows (identified in Exp-NoCor) from
different OSSEs. It confirms that in all OSSEs, the posterior uncertainties
for clumps with larger emissions are smaller than those with lower
emissions. Within a given bin of clump annual emission, the posterior
uncertainties from the various OSSEs are very similar, even though they are
obtained with different hypotheses regarding the temporal auto-correlation
in the prior uncertainty. The interpretation is that, for the inversion of
the 3 h emissions before a given satellite overpass, most of the constraint
is imposed by the direct satellite observations during this overpass. These
observations are independent on different days, and the constraints on
different days are not strongly crossed even when errors in the prior
estimate are highly correlated in time. However, although small, the impact
of temporal auto-correlations in the prior uncertainties can be seen. For
example, the posterior uncertainties in ASS (SCS) are systematically smaller
than those in AMS (MCS), which confirms that the capability of the inversion
system to use the information from observations from previous or subsequent
days to reduce the posterior uncertainties increases with the temporal
auto-correlations. In SectCS, the posterior uncertainties are smaller than
those in MCS and SCS in most regions (Fig. S5), due to the fact that the
uncertainty in industrial emissions has a long temporal auto-correlation
(<inline-formula><mml:math id="M247" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="italic">τ</mml:mi><mml:mn mathvariant="normal">2</mml:mn></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">180</mml:mn></mml:mrow></mml:math></inline-formula> d).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2" specific-use="star"><?xmltex \currentcnt{2}?><label>Figure 2</label><caption><p id="d1e4567"><bold>(a)</bold> Number of 08:30–11:30 time windows within a year for which the 3 h emissions are constrained with a posterior uncertainty less than 20 % (N20) in the Exp-NoCor experiment. The results are binned according to clump annual emission with bin limits given on the <inline-formula><mml:math id="M248" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis of the figure. Dots and error bars are the median and interquartile range of N20 for all clumps within the emission bin. Numbers at the figure top indicate the number of clumps and the percentage of clump emission within each bin. <bold>(b)</bold> Number of 08:30–11:30 time windows (color) within a year for which the 3 h emissions are constrained with a posterior uncertainty less than a given threshold (<inline-formula><mml:math id="M249" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axis) in the Exp-NoCor experiment.</p></caption>
          <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020-f02.png"/>

        </fig>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><?xmltex \currentcnt{3}?><label>Figure 3</label><caption><p id="d1e4597">Distribution of the posterior uncertainty in the 3 h mean emissions during the 08:30–11:30 time windows (for which the posterior uncertainty in 3 h mean emissions are smaller than 20 % in Exp-NoCor) obtained with
different OSSEs. Dots and error bars are the median and interquartile range.
The results are binned according to the clump annual emission with bin
limits given on the <inline-formula><mml:math id="M250" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis of the figure. Numbers at the figure top indicate the number of clumps and the percentage of clump emission within each bin.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020-f03.png"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS3">
  <label>3.3</label><?xmltex \opttitle{Potential of space observations for monitoring daily {$\protect\chem{CO_{2}}$} emissions}?><title>Potential of space observations for monitoring daily <inline-formula><mml:math id="M251" 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> emissions</title>
      <p id="d1e4633">In previous sections, we analyzed the uncertainty reduction and the
posterior uncertainty for the 3 h emissions that generate the atmospheric
plume observed from space at 11:30. We now analyze the potential to monitor
the daily emission, relying on the extrapolation of constraints on emissions
between 08:30 and 11:30 using temporal auto-correlation of the prior
uncertainties in step 2 of the inversion (Sect. 2.7.2). Figure 4 shows the distribution of the number of days when the posterior uncertainties in daily emissions are smaller than 20 % (D20) for the same bins of emission clumps as in the previous section. Similar to the distribution of N20, clumps with small emission budgets tend to have lower D20 values than those with large budgets, due to having smaller signal-to-noise ratios for clumps with smaller emissions. The D20 values also strongly depend on the temporal auto-correlation in the prior uncertainty. When no correlation (Exp-NoCor) or short correlation (MCS) are assumed, D20 remains zero even for the largest clumps, since most of the daily emissions are disconnected from the 3 h emissions that are constrained by the satellite observation and keep
on bearing the large prior uncertainties associated with the Exp-NoCor and
MCS scenarios. When significant temporal auto-correlations (e.g., in the case
of AMS, ASS and SCS) are assumed, the results get better and the posterior
uncertainties for the daily emissions become less than 20 % for more than
100 d for clumps emitting more than 5 MtC yr<inline-formula><mml:math id="M252" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. At regional scale
(Fig. S6), the distribution of D20 values shows a similar pattern to N20: North America, South America and Africa have larger D20 values than the Middle East and Asia for same bin of clump annual emission. But the distribution D20 values in SectCS have large regional variations, reflecting the regional differences in the share of emissions from different sectors.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4" specific-use="star"><?xmltex \currentcnt{4}?><label>Figure 4</label><caption><p id="d1e4650">Number of days within the year when the posterior uncertainty of daily emissions is smaller than 20 % (D20). The results are binned according to the clump annual emission with bin limits given on the <inline-formula><mml:math id="M253" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis of the figure. Note that the median values of D20 for all clumps in Exp-NoCor and in MCS, for clumps whose annual emissions are between 0.5 and 1 MtC in AMS, ASS and SCS, and for clumps whose emissions are below 10 MtC in SectCS, are all zero, so that the dots in these cases are not visible on the <inline-formula><mml:math id="M254" display="inline"><mml:mi>y</mml:mi></mml:math></inline-formula> axis with log scale. The dots and error bars are the median and interquartile range of D10 for all clumps within the emission bin. Numbers at the figure top indicate the number of clumps and the percentage of clump emission within each bin.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020-f04.png"/>

        </fig>

</sec>
<sec id="Ch1.S3.SS4">
  <label>3.4</label><?xmltex \opttitle{Potential of space observations for monitoring annual {$\protect\chem{CO_{2}}$} emissions}?><title>Potential of space observations for monitoring annual <inline-formula><mml:math id="M255" 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> emissions</title>
      <p id="d1e4693">We now analyze the results for the annual emissions, allowed again by the
derivation of the posterior uncertainty covariance matrix <inline-formula><mml:math id="M256" display="inline"><mml:mi mathvariant="bold">A</mml:mi></mml:math></inline-formula> for individual clumps in step 2 of the inversion, and thus the aggregation of the posterior uncertainties in time. Figure 5 shows the posterior uncertainties in annual emissions from the OSSEs. When we assume that there is no temporal
auto-correlations in the prior uncertainties, the uncertainties obtained
from the inversions remain very close to the prior uncertainties (30 %)
for all emission bins since the information from the few well-constrained
08:30–11:30 time windows within the year is not extrapolated to the huge
unobserved fraction of the total annual emission over the year. The benefit
of satellite observations becomes apparent when assuming that the prior
uncertainties have temporal auto-correlations. Similar to the posterior
uncertainties for 3 h emissions during 08:30–11:30, the posterior
uncertainties in annual emissions are smaller in the OSSEs where the prior
uncertainties have stronger temporal auto-correlation. This indicates that
temporal auto-correlations help to extrapolate the information on the
emissions from the satellite passes over a given clump to emissions during
other hours and days when there are no direct observations. Small clumps tend
to have a larger relative posterior uncertainty in annual emissions than
large clumps even when temporal error correlations are accounted for. The
posterior uncertainties in the annual emissions of large cities with annual
emission <inline-formula><mml:math id="M257" display="inline"><mml:mrow><mml:mo>&gt;</mml:mo><mml:mn mathvariant="normal">5</mml:mn></mml:mrow></mml:math></inline-formula> MtC yr<inline-formula><mml:math id="M258" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> can be constrained to better than
20 % in AMS, SCS and SectCS, and to better than 10 % in ASS. On the
other hand, the posterior uncertainties for small emission clumps with
annual emissions <inline-formula><mml:math id="M259" display="inline"><mml:mrow><mml:mo>&lt;</mml:mo><mml:mn mathvariant="normal">0.5</mml:mn></mml:mrow></mml:math></inline-formula> MtC yr<inline-formula><mml:math id="M260" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> are always larger than 15 %,
regardless of the temporal auto-correlations in prior uncertainties.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5" specific-use="star"><?xmltex \currentcnt{5}?><label>Figure 5</label><caption><p id="d1e4749">Distribution of the posterior uncertainties in annual <inline-formula><mml:math id="M261" 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> emissions for different OSSEs. The results are binned according to the clump annual emission with bin limits given on the <inline-formula><mml:math id="M262" display="inline"><mml:mi>x</mml:mi></mml:math></inline-formula> axis of the figure. Dots and
error bars are the median and interquartile range of posterior uncertainty.
Numbers at the figure top indicate the number of clumps and the percentage
of clump emission within that bin.</p></caption>
          <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020-f05.png"/>

        </fig>

</sec>
</sec>
<?pagebreak page5824?><sec id="Ch1.S4" sec-type="conclusions">
  <label>4</label><title>Discussion and conclusions</title>
      <p id="d1e4785">PMIF provides information on the potential of space-borne imagery to constrain <inline-formula><mml:math id="M263" 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> emissions from emission clumps over the globe from scales of a few hours to the annual scale. It uses a simple Gaussian plume model to relate the emissions and the <inline-formula><mml:math id="M264" 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> plumes. This is a strong simplification of the physics which impacts the range of uncertainties that can be accounted for in the inversion problem, but a preliminary evaluation against a more complex setup (that of Broquet et al., 2018) indicates that it provides the correct order of magnitude for the uncertainties in the inverted emissions for an individual city: Paris.</p>
      <p id="d1e4810">In this study, we focused on the projection of uncertainties in satellite
observations on the uncertainty of inverted emissions. Some sources of
uncertainties that could have some impacts on the inversions when dealing
with real data are ignored. Firstly, the plumes generated by the Gaussian
plume model are straight along the wind direction at the source pixel. As a
result, we allow the plumes from nearby clumps to potentially cross each
other, but these plumes will systematically diverge over long distances. The
Gaussian plume model cannot reproduce plumes overlapping along the
atmospheric circulation like Eulerian transport models. In this sense, the
overlapping effect of plumes can be underestimated in PMIF. In a realistic
situation of atmospheric transport, if plumes from multiple clumps overlap
very often, the inversion performance for individual clumps will be degraded
since it will have difficulties accurately attributing the <inline-formula><mml:math id="M265" 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>
signals to individual clumps. Furthermore, we assume that the Gaussian plume
model can perfectly link the emissions and <inline-formula><mml:math id="M266" 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> and ignore the
transport model error. If forced with erroneous wind fields, the simulation
of <inline-formula><mml:math id="M267" 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> plumes can have the wrong shape and location and thus generate
large uncertainties in the inversions. In the inversion with actual
<inline-formula><mml:math id="M268" 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> observations from OCO-2, Nassar et al. (2017) allowed the wind direction to change from the wind re-analysis used to force the Gaussian plume model, if it improved the fit between simulated plumes and the observed signals. Reuter et al. (2019) and Kuhlmann et al. (2019) showed that the
co-located <inline-formula><mml:math id="M269" 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> satellite observations could help to detect and
constrain the location and shape of <inline-formula><mml:math id="M270" 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> plumes. The transport model
error may be partly reduced by incorporating additional information from
other tracers when fitting the model to real data, but it is unknown to
what extent these additional constraints are useful to improve the inversion
of <inline-formula><mml:math id="M271" 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> emissions from cities and point sources. With the current design of PMIF, the impact of transport error is hard<?pagebreak page5826?> to evaluate. Secondly, we ignore systematic measurement errors from the <inline-formula><mml:math id="M272" 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> imagery. Broquet et al. (2018) showed that systematic error could hamper the ability of the inversion system to reduce the errors in the emissions estimates. Thirdly, we neglect the impact of uncertainties in diffuse fossil fuel <inline-formula><mml:math id="M273" 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> emissions (outside clumps) and non-fossil <inline-formula><mml:math id="M274" 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> fluxes (within and outside clumps), the latter including net ecosystem exchange (NEE) from the terrestrial biosphere, the <inline-formula><mml:math id="M275" 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> emitted by the burning of biofuel, the respiration from humans and animals (Ciais et al., 2020), and the net <inline-formula><mml:math id="M276" 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> fluxes between the atmosphere and ocean. For example, the signals from terrestrial NEE can be strong during the growing season, and the
signals from ocean <inline-formula><mml:math id="M277" 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> fluxes may have a critical impact on the overall <inline-formula><mml:math id="M278" 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> patterns in proximity to coastlines. In principle, the signals of diffuse fossil fuel <inline-formula><mml:math id="M279" 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> emissions and non-fossil <inline-formula><mml:math id="M280" 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> fluxes outside the clumps can be potentially filtered by removing the local background <inline-formula><mml:math id="M281" 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> field to extract plumes generated only by emissions from clumps (Kuhlmann et al., 2019; Reuter et al., 2019; Ye et al., 2020; Zheng et al., 2020). The non-fossil <inline-formula><mml:math id="M282" 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> fluxes within clumps vary from clump to clump and could contribute a non-negligible fraction of the total <inline-formula><mml:math id="M283" 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> fluxes in many clumps (Bréon et al., 2015; Ciais et al., 2020; Wu et al., 2018). The satellite observations
alone cannot effectively differentiate the fossil fuel <inline-formula><mml:math id="M284" 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> emissions
and the non-fossil <inline-formula><mml:math id="M285" 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> fluxes within clumps. Fourthly, the PMIF system controls the scaling factors for the mean emissions of daily 3 and 21 h windows and for each clump, ignoring uncertainties in the spatial
distribution and temporal profile of the emissions (described by the
operator <inline-formula><mml:math id="M286" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">inventory</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula>) within the clumps and over the time windows. Such uncertainties are called aggregation errors (Wang et al., 2017; Wu et al., 2011). However, Broquet et al. (2018) compared the results of
inversions using the realistic spatial distribution of emissions and using a
homogenous one over two discs with a different radius for <inline-formula><mml:math id="M287" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">inventory</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> and
found that having imperfect spatial distribution of emissions to model
<inline-formula><mml:math id="M288" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="bold">M</mml:mi><mml:mi mathvariant="normal">inventory</mml:mi></mml:msub></mml:mrow></mml:math></inline-formula> (thus the aggregation error) only has a small impact on the
uncertainties and errors in the inverted emissions. Future developments in
PMIF should attempt to quantify the impacts of such sources of
uncertainties, while keeping its power of constraining the emissions from a
large range of sources with global coverage.</p>
      <p id="d1e5081">Although it ignores the sources of uncertainties listed above, the current
PMIF can still be used to investigate the impacts of some key parameters of
the inversion problem and to allow, for the first time, a first-order
extrapolation of the results from single-city studies to all significant
emission clumps over the globe and under a full range of meteorological
conditions during a year.</p>
      <p id="d1e5084">The key result summarized in Fig. 2 is that using a single CO2M satellite,
only the clumps with annual budget higher than 2 MtC yr<inline-formula><mml:math id="M289" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (e.g., Manchester, UK, Boston, USA and Chongqing, China) can potentially be well
constrained with N20 being larger than 10 within a year. However, there are large variations in the N20 values for clumps with such levels of emission. Figure 6a and b show the maps of the number of observations within each <inline-formula><mml:math id="M290" display="inline"><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> grid cell during 1 year in the USA and China, which is an indicator for the frequency of clear-sky days: the larger the number of observations, the higher the frequency of clear-sky days. It is clearly seen in Fig. 6c and d that the clumps in
southern China have low N20 values when they are located in areas with a low frequency of clear-sky days. For clumps that have emissions between 2 and 5 MtC yr<inline-formula><mml:math id="M291" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, N20 values are below 10 d in a cloudy/hazy region like southeastern China and are close to 30 d in a clear-sky region like the western coast of the USA. These results illustrate the dependence of the potential of satellite observations to constrain emissions on the frequency of clear-sky conditions. The relative uncertainty in the inversion of the emissions from a clump is primarily driven by the budget of these emissions, and by the wind speed (as illustrated by Fig. 1). The frequency of clear-sky days modulates the number of direct observations of the plume from a clump and thus the number of days for which the inversion can decrease the uncertainty when ignoring temporal auto-correlations in the prior uncertainty in Exp-NoCor. The frequency of clear-sky days, together with the emission rate and wind speed, are the main drivers of the posterior
uncertainty in daily to annual emissions when accounting for temporal
auto-correlations in the prior uncertainty.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F6" specific-use="star"><?xmltex \currentcnt{6}?><label>Figure 6</label><caption><p id="d1e5134">Number of observations in <inline-formula><mml:math id="M292" display="inline"><mml:mrow><mml:mn mathvariant="normal">2</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup><mml:mo>×</mml:mo><mml:mn mathvariant="normal">2</mml:mn><mml:msup><mml:mi/><mml:mo>∘</mml:mo></mml:msup></mml:mrow></mml:math></inline-formula> grid cells during 1 year <bold>(a, b)</bold> and N20 values <bold>(c, d)</bold>.</p></caption>
        <?xmltex \igopts{width=369.885827pt}?><graphic xlink:href="https://gmd.copernicus.org/articles/13/5813/2020/gmd-13-5813-2020-f06.png"/>

      </fig>

      <p id="d1e5169">We showed that one CO2M imager can provide a direct constraint for the
estimate of emissions from clumps with emissions larger than 2 MtC yr<inline-formula><mml:math id="M293" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, but over limited periods only. N20 is smaller than 25 for most clumps, indicating that even for emissions during 08:30–11:30, one cannot expect more than 25 d when the CO2M observations sample the plumes from clumps with a sufficient number of observations (Fig. 2) during 1 year. The use of a constellation of CO2M satellites in the current plan could potentially improve the frequency of good samplings. Imaging from geostationary orbit (GEO) imagers like NASA's GeoCarb mission (O'Brien et al., 2016; Polonsky et al., 2014) could offer sampling during different periods within a day to constrain the diurnal profile of emissions. Highly
elliptical orbit (HEO) imagers could also provide observations at northern
high latitudes with a similar high frequency to GEO (Nassar et al., 2014). However, even though multiple space-borne platforms can sample the plumes more frequently, the satellites using passive sensors like that planned for CO2M can never sample the plumes under cloudy/hazy conditions.</p>
      <p id="d1e5184">We also investigated the possibility of extrapolating the information
obtained from the time windows for which the emissions are constrained by
satellite observations to estimate emissions on other hours, days and
throughout a year. Such an extrapolation relies on the model of the emission
inventories used as a prior of PMIF, that is, in the framework of PMIF, the
temporal auto-correlation of the uncertainty of prior emissions. The
analysis of posterior uncertainties in the 3 h mean emissions, in daily
emissions and in annual<?pagebreak page5827?> emissions all show that the configuration of this
temporal auto-correlation has a large impact on the inversion results. For
example, posterior uncertainties in annual emissions range from less than
10 % with strong auto-correlation (ASS) to 25 % with medium
auto-correlation (MCS) for clumps with emissions higher than 2 MtC yr<inline-formula><mml:math id="M294" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>. The orders of magnitude in the posterior uncertainty will be critical to the objective assessment of annual emissions. However, since state-of-the-art emission products rarely report their uncertainties and temporal auto-correlations (Andres et al., 2016; Gurney et al., 2019), it is difficult to exclude any configuration of OSSEs in this study. The strong impact of the prior uncertainty on the inversion results thus highlights the priority of future research to systematically assess the uncertainty, especially the temporal error co-variances, in the emission products.</p>
      <p id="d1e5199">Even if emissions can be effectively constrained by CO2M for clumps whose
emissions are larger than 2 MtC yr<inline-formula><mml:math id="M295" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, the sum of annual emission budgets from these large clumps account only for 54 % of the total <inline-formula><mml:math id="M296" 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> clump emissions and for 36 % of the total global fossil fuel <inline-formula><mml:math id="M297" 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> emissions (accounting for diffuse emissions outside the clumps), according to the clump definition of Wang et al. (2019) and the ODIAC
emission map. For a specific country, clumps with emissions larger than 2 MtC yr<inline-formula><mml:math id="M298" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> typically represent less than 50 % of the total national emissions (accounting for diffuse emissions outside the clumps). It thus shows the difficulty of using a single CO2M imager as the only source of
information to constrain national emissions. This limitation of a single
CO2M imager calls for innovations to integrate other types of observations
in inversion systems to improve the ability to estimate emissions at both
city scale (Lauvaux et al., 2016; Sargent et al., 2018; Staufer et al., 2016) and larger spatial scales (Palmer et al., 2018; Wang et al., 2018a).</p><?xmltex \hack{\clearpage}?>
</sec>

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

<?pagebreak page5828?><app id="App1.Ch1.S1">
  <?xmltex \currentcnt{A}?><label>Appendix A</label><title>Acronyms</title>
      <p id="d1e5261"><table-wrap id="Taba" position="anchor"><oasis:table><oasis:tgroup cols="2">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="left"/>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">AMS:</oasis:entry>
         <oasis:entry colname="col2">Annual component and moderately correlated sub-annual component</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">ASS:</oasis:entry>
         <oasis:entry colname="col2">Annual component and strongly correlated sub-annual component</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">CDIAC:</oasis:entry>
         <oasis:entry colname="col2">Carbon Dioxide Information Analysis Center</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">CNES:</oasis:entry>
         <oasis:entry colname="col2">Centre National d'Etudes Spatiales</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">CO2M:</oasis:entry>
         <oasis:entry colname="col2">Copernicus Anthropogenic Carbon Dioxide Monitoring</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">D20:</oasis:entry>
         <oasis:entry colname="col2">Number of days within the year when the posterior uncertainty of daily emissions is smaller than 20 %</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">ECMWF:</oasis:entry>
         <oasis:entry colname="col2">European Centre for Medium-Range Weather Forecasts</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">ESA:</oasis:entry>
         <oasis:entry colname="col2">European Space Agency</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">EUMETSAT:</oasis:entry>
         <oasis:entry colname="col2">European Organisation for the Exploitation of Meteorological Satellites</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">GOSAT:</oasis:entry>
         <oasis:entry colname="col2">Greenhouse Gases Observing Satellite</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">MCS:</oasis:entry>
         <oasis:entry colname="col2">Moderately correlated sub-annual component</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">N20:</oasis:entry>
         <oasis:entry colname="col2">Number of 08:30–11:30 time windows per clump for which the posterior uncertainty of 3 h mean</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">emissions is smaller than 20 %</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">NoCor:</oasis:entry>
         <oasis:entry colname="col2">No temporal auto-correlation</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">OCO:</oasis:entry>
         <oasis:entry colname="col2">Orbiting Carbon Observatory</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">ODIAC:</oasis:entry>
         <oasis:entry colname="col2">Open-source Data Inventory for Anthropogenic <inline-formula><mml:math id="M299" 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></oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">OSSE:</oasis:entry>
         <oasis:entry colname="col2">Observing System Simulation Experiment</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">PMIF:</oasis:entry>
         <oasis:entry colname="col2">Plume Monitoring Inversion Framework</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">SCS:</oasis:entry>
         <oasis:entry colname="col2">Strongly correlated sub-annual component</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">SectCS:</oasis:entry>
         <oasis:entry colname="col2">Sector-dependent correlated sub-annual component</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">SZA:</oasis:entry>
         <oasis:entry colname="col2">Solar zenith angle</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">TIMES:</oasis:entry>
         <oasis:entry colname="col2">Temporal Improvements for Modeling Emissions by Scaling</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1"><inline-formula><mml:math id="M300" 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>:</oasis:entry>
         <oasis:entry colname="col2">Vertically integrated columns of dry-air mole fractions of <inline-formula><mml:math id="M301" 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></oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table></table-wrap></p><?xmltex \hack{\clearpage}?>
</app>
  </app-group><notes notes-type="codeavailability"><title>Code availability</title>

      <p id="d1e5518">The source code for PMIFv1.0 is included in the Supplement. To run PMIF, some input files are needed. The ODIAC inventory is available at
<ext-link xlink:href="https://doi.org/10.17595/20170411.001" ext-link-type="DOI">10.17595/20170411.001</ext-link> (Oda and Maksyutov, 2015). The clump dataset is available at
<ext-link xlink:href="https://doi.org/10.6084/m9.figshare.7217726.v1" ext-link-type="DOI">10.6084/m9.figshare.7217726.v1</ext-link> (Wang et al., 2018b). The list of clump
information (e.g., index, latitude and longitude of the center), which is
also needed as an input, is included in the Supplement. The wind fields from
CCMP are available at <uri>http://www.remss.com/measurements/ccmp/</uri> (last access: 26 July 2017, Remote Sensing Systems, 2017, <ext-link xlink:href="https://doi.org/10.1175/2010BAMS2946.1" ext-link-type="DOI">10.1175/2010BAMS2946.1</ext-link>, Atlas et al., 2011). EDGAR v4.3.2
emission maps are needed to run the SectCS inversion and are available at
<uri>https://edgar.jrc.ec.europa.eu/overview.php?v=432_GHG</uri> (last access: 25 July 2019, JRC, 2019, additional information can be found at <ext-link xlink:href="https://doi.org/10.5194/essd-11-959-2019" ext-link-type="DOI">10.5194/essd-11-959-2019</ext-link>, Janssens-Maenhout et al., 2019).</p>
  </notes><app-group>
        <supplementary-material position="anchor"><p id="d1e5540">The supplement related to this article is available online at: <inline-supplementary-material xlink:href="https://doi.org/10.5194/gmd-13-5813-2020-supplement" xlink:title="zip">https://doi.org/10.5194/gmd-13-5813-2020-supplement</inline-supplementary-material>.</p></supplementary-material>
        </app-group><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e5549">PC, GB and FMB designed the research. YW and FL developed the PMIF code and performed the analysis. MB and MR simulated the satellite sampling and random measurement noise for CarbonSat and CO2M imagers. YW, GB, FMB, FL, MB, MR, YM, AL, GLM, BZ and PC wrote the paper.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e5555">The authors declare that they have no conflict of interest.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e5561">This work was mainly conducted and funded in the frame of the ESA. It also received support from the French National Research Agency (ANR). Yilong Wang also acknowledges support from National Key Research and Development Program of China. We would like to thank Bernard Pinty for providing the vision of a <inline-formula><mml:math id="M302" 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> Monitoring and Verification Support (MVS) Capacity within the framework of the EU's Copernicus Programme.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e5577">This research has been supported by the ESA (project no. 4000120184/17/NL/FF/mg), the French National Research Agency (ANR)'s program “Chaires Industrielles 2017” through the TRACE Industrial Chair (UVSQ/CEA/CNRS/Thales Alenia Space/TOTAL/SUEZ) (grant no. ANR-17-CHIN-0004), and the National Key Research and Development Program of China (grant no. 2017YFA0605303).</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e5583">This paper was edited by Havala Pye and reviewed by two anonymous referees.</p>
  </notes><ref-list>
    <title>References</title>

      <ref id="bib1.bib1"><label>1</label><?label 1?><mixed-citation>Andres, R. J., Gregg, J. S., Losey, L., Marland, G., and Boden, T. A.:
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    <!--<article-title-html>PMIF v1.0: assessing the potential of satellite observations to constrain CO<sub>2</sub> emissions from large cities and point sources over the globe using synthetic data</article-title-html>
<abstract-html><p>This study assesses the potential of satellite imagery of vertically integrated columns of dry-air mole fractions of CO<sub>2</sub> (XCO<sub>2</sub>) to constrain the emissions from cities and power plants (called emission clumps) over the whole globe during 1 year. The imagery is simulated for one imager of the Copernicus mission on Anthropogenic Carbon Dioxide Monitoring (CO2M) planned by the European Space Agency and the European Commission. The width of the swath of the CO2M instruments is about
300&thinsp;km and the ground horizontal resolution is about 2&thinsp;km resolution. A
Plume Monitoring Inversion Framework (PMIF) is developed, relying on a
Gaussian plume model to simulate the XCO<sub>2</sub> plumes of each emission clump and on a combination of overlapping assimilation windows to solve for the inversion problem. The inversion solves for the 3&thinsp;h mean emissions (during 08:30–11:30 local time) before satellite overpasses and for the mean emissions during other hours of the day (over the aggregation between
00:00–08:30 and 11:30–00:00) for each clump and for the 366&thinsp;d of the year. Our analysis focuses on the derivation of the uncertainty in the inversion estimates (the <q>posterior uncertainty</q>) of the clump emissions. A comparison of the results obtained with PMIF and those from a previous study using a complex 3-D Eulerian transport model for a single city (Paris) shows that the PMIF system provides the correct order of magnitude for the uncertainty reduction of emission estimates (i.e., the relative difference between the prior and posterior uncertainties). Beyond the one city or few large cities studied by previous studies, our results provide, for the first time, the global statistics of the uncertainty reduction of emissions for the full range of global clumps (differing in emission rate and spread, and distance from other major clumps) and meteorological conditions. We show that only the clumps with an annual emission budget higher than 2&thinsp;MtC&thinsp;yr<sup>−1</sup> can potentially have their emissions between 08:30 and 11:30 constrained with a posterior uncertainty smaller than 20&thinsp;% for more than 10 times within 1 year (ignoring the potential to cross or extrapolate information between 08:30–11:30 time windows on different days). The PMIF inversion results are also aggregated in time to investigate the potential of CO2M observations to constrain daily and annual emissions, relying on the extrapolation of information obtained for 08:30–11:30 time windows during days when clouds and aerosols do not mask the plumes, based on various assumptions regarding the temporal auto-correlations of the uncertainties in the emission estimates that are used as a prior knowledge in the Bayesian framework of PMIF. We show that the posterior uncertainties of daily and annual emissions are highly dependent on these temporal auto-correlations, stressing the need for systematic assessment of the sources of uncertainty in the
spatiotemporally resolved emission inventories used as prior estimates in
the inversions. We highlight the difficulty in constraining the total budget of
CO<sub>2</sub> emissions from all the cities and power plants within a country or over the globe with satellite XCO<sub>2</sub> measurements only, and calls for integrated inversion systems that exploit multiple types of measurements.</p></abstract-html>
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