Local and regional enhancements of CH₄, CO, and CO₂ inferred from TCCON column measurements

Creators: Mottungan, Kavitha^{1, 2}; Roychoudhury, Chayan¹; Brocchi, Vanessa^{1, 3}; Gaubert, Benjamin⁴; Tang, Wenfu⁴; Mirrezaei, Mohammad Amin¹; McKinnon, John¹; Guo, Yafang¹; Griffith, David W. T.⁵; Feist, Dietrich G.^{6, 7, 8}; Morino, Isamu⁹; Sha, Mahesh K.¹⁰; Dubey, Manvendra K.¹¹; De Mazière, Martine¹⁰; Deutscher, Nicholas M.⁵; Wennberg, Paul O.¹²; Sussmann, Ralf¹³; Kivi, Rigel¹⁴; Goo, Tae-Young¹⁵; Velazco, Voltaire A.¹⁶; Wang, Wei¹⁷; Arellano Jr., Avelino F.¹

1. University of Arizona
2. National Physical Laboratory
3. Atmo Auvergne-Rhône-Alpes
4. National Center for Atmospheric Research
5. University of Wollongong
6. German Aerospace Center
7. Ludwig-Maximilians-Universität München
8. Max Planck Institute for Biogeochemistry
9. National Institute for Environmental Studies
10. Royal Belgian Institute for Space Aeronomy
11. Los Alamos National Laboratory
12. California Institute of Technology
13. Karlsruhe Institute of Technology
14. Finnish Meteorological Institute
15. National Institute of Meteorological Sciences
16. German Meteorological Service
17. Anhui Institute of Optics and Fine Mechanics

Abstract

In this study, we demonstrate the utility of available correlative measurements of carbon species to identify regional and local air mass characteristics as well as their associated source types. In particular, we combine different regression techniques and enhancement ratio algorithms with carbon monoxide (CO), carbon dioxide (CO₂), and methane (CH₄) total column abundance from 11 sites of the Total Carbon Column Observing Network (TCCON) to infer relative contributions of regional and local sources to each of these sites. The enhancement ratios provide a viable alternative to univariate measures of relationships between the trace gases that are insufficient in capturing source-type and transport signatures. Regional enhancements are estimated from the difference between bivariate regressions across a specific time window of observed total abundance of these species (BERr for bulk enhancement regression ratio) and inferred anomalies (AERr for anomaly enhancement regression ratio) associated with a site-specific background. Since BERr and AERr represent the bulk and local species enhancement ratio, respectively, its difference simply represents the site-specific regional component of these ratios. We can then compare these enhancements for CO₂ and CH₄ with CO to differentiate between combustion and non-combustion air masses. Our results show that while the regional and local influences in enhancements vary across sites, dominant characteristics are found to be consistent with previous studies over these sites and with bottom-up anthropogenic and fire emission inventories. The site in Pasadena shows a dominant local influence (> 60 %) across all species enhancement ratios, which appear to come from a mixture of biospheric and combustion activities. In contrast, Anmyeondo shows more regionally influenced (> 60 %) air masses associated with high-temperature and/or biofuel combustion activities. Ascension Island appears to only show a large regional influence (> 80 %) on CO CO₂ and CO CH₄, which is indicative of transported and combustion-related CO from the nearby African region, consistent with a sharp rise in column CO (3.51 ± 0.43 % ppb yr⁻¹) at this site. These methods have important applications to source analysis using spaceborne column retrievals of these species.

Copyright and License

Published by Copernicus Publications on behalf of the European Geosciences Union.

Acknowledgement

This research work is supported by NASA ACMAP (grant no. 80NSSC19K0947). Wenfu Tang is supported by the National Center for Atmospheric Research (NCAR) Advanced Study Program Postdoctoral Fellowship. The TCCON data for total column measurements of CO, CO₂, and CH₄ at Pasadena, Ascension, Manaus, Garmisch, Sodankylä, Anmyeondo, Burgos, Hefei, Darwin, Wollongong, and Réunion were obtained from the TCCON Data Archive (GGG 2014), hosted by CaltechDATA at https://tccondata.org. The Ascension Island TCCON station has been supported by the European Space Agency (ESA) under grant no. 4000120088/17/I-EF and by the German Bundesministerium für Wirtschaft und Energie (BMWi) under grant nos. 50EE1711C and 50EE1711E. We thank the ESA Ariane Tracking Station at North East Bay, Ascension Island, for hosting and local support. The TCCON site at Réunion has been operated by the Royal Belgian Institute for Space Aeronomy with financial support since 2014 by the EU project ICOS-Inwire (grant no. ID 313169), the ministerial decree for ICOS (FR/35/IC1 to FR/35/C6), ESFRI-FED ICOS-BE project (EF/211/ICOS-BE), and local activities supported by LACy/UMR8105 and by OSU-R/UMS3365 – Université de La Réunion. The Burgos TCCON site is supported in part by the GOSAT series project, with local support from the Energy Development Corp., Philippines. We also acknowledge the Emission of Atmospheric Compounds and Compilation of the Ancillary Data (ECCAD, https://eccad.sedoo.fr) for anthropogenic and biomass burning emission data of CO, CO₂, and CH₄ from the inventories of Copernicus Atmosphere Monitoring Service (CAMS v4.1) and Global Fire Emission Database (GFED4) during the 2012–2019 period. This material is partly based upon work supported by the US NSF NCAR, which is a major facility sponsored by the National Science Foundation under cooperative agreement no. 1852977.

Funding

This research has been supported by the National Aeronautics and Space Administration (grant no. 80NSSC19K0947).

Contributions

Conceptualization: AFA Jr., WT; investigation: KM, VB, CR, and AFA Jr.; methodology: KM, VB, AFA Jr., CR; formal analysis: KM, VB, AFA Jr., CR; data curation: KM, CR, DWTG, DGF, IM, MKS, MKD, MDM, NMD, POW, RS, RK, TYG, VAV, WW; validation: KM, CR; visualization: KM, CR; supervision: AFA Jr.; writing (original draft preparation): KM, AFA Jr.; writing (review and editing): BG, WT, CR, MAM, JM, YG, MKS, VAV, and AFA Jr.

Data Availability

The TCCON data were obtained from the TCCON Data Archive, hosted by CaltechDATA at https://tccondata.org/2014 (last access: 6 June 2023). The DOI for the entire 2014 dataset is https://doi.org/10.14291/TCCON.GGG2014 (Total Carbon Column Observing Network (TCCON) Team, 2017). The DOIs for each site are provided in Table 1. Supporting datasets were obtained from the following: Emissions of atmospheric Compounds and Compilation of the Ancillary Data (ECCAD, 2023, https://eccad.sedoo.fr/) for CAMS v4.1 and GFED4, MOPITT from NASA through the Earthdata portal at https://doi.org/10.5067/TERRA/MOPITT/MOP03JM_L3.008 (NASA/LARC/SD/ASDC, 2000), GOSAT-1 from NIES at https://data2.gosat.nies.go.jp (NIES, 2023), and OCO-2 from NASA through the Goddard Earth Science Data and Information Services Center for registered users.

Conflict of Interest

At least one of the (co-)authors is a member of the editorial board of Atmospheric Measurement Techniques. The peer-review process was guided by an independent editor, and the authors also have no other competing interests to declare.

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Local and regional enhancements of CH₄, CO, and CO₂ inferred from TCCON column measurements

Abstract

Copyright and License

Acknowledgement

Funding

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Data Availability

Conflict of Interest

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