Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021
<p>Volatile organic compounds (VOCs) are key precursors of particulate matter and tropospheric ozone. Although the terrestrial biosphere is by far the largest source of VOCs into the atmosphere, the emissions of biogenic VOCs remain poorly constrained at the regional scale. In this work, we de...
| Main Authors: | , , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2024-01-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://acp.copernicus.org/articles/24/449/2024/acp-24-449-2024.pdf |
| _version_ | 1797357461861040128 |
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| author | G.-M. Oomen J.-F. Müller T. Stavrakou I. De Smedt T. Blumenstock R. Kivi M. Makarova M. Palm A. Röhling Y. Té C. Vigouroux M. M. Friedrich U. Frieß F. Hendrick A. Merlaud A. Piters A. Richter M. Van Roozendael T. Wagner |
| author_facet | G.-M. Oomen J.-F. Müller T. Stavrakou I. De Smedt T. Blumenstock R. Kivi M. Makarova M. Palm A. Röhling Y. Té C. Vigouroux M. M. Friedrich U. Frieß F. Hendrick A. Merlaud A. Piters A. Richter M. Van Roozendael T. Wagner |
| author_sort | G.-M. Oomen |
| collection | DOAJ |
| description | <p>Volatile organic compounds (VOCs) are key precursors of particulate matter and tropospheric ozone. Although the terrestrial biosphere is by far the largest source of VOCs into the atmosphere, the emissions of biogenic VOCs remain poorly constrained at the regional scale. In this work, we derive top-down biogenic emissions over Europe using weekly averaged TROPOMI formaldehyde (HCHO) data from 2018 to 2021. The systematic bias of the TROPOMI HCHO columns is characterized and corrected for based on comparisons with FTIR data at seven European stations. The top-down fluxes of biogenic, pyrogenic, and anthropogenic VOC sources are optimized using an inversion framework based on the MAGRITTEv1.1 chemistry transport model and its adjoint. The inversion leads to strongly increased isoprene emissions with respect to the MEGAN–MOHYCAN inventory over the model domain (from 8.1 to 18.5 <span class="inline-formula">Tg yr<sup>−1</sup></span>), which is driven by the high observed TROPOMI HCHO columns in southern Europe. The impact of the inversion on biomass burning VOCs (<span class="inline-formula">+</span>13 %) and anthropogenic VOCs (<span class="inline-formula">−</span>17 %) is moderate. An evaluation of the optimized HCHO distribution against ground-based remote sensing (FTIR and MAX-DOAS) and in situ data provides generally improved agreement at stations below about 50<span class="inline-formula"><sup>∘</sup></span> N but indicates overestimated emissions in northern Scandinavia. Sensitivity inversions show that the top-down emissions are robust with respect to changes in the inversion settings and in the model chemical mechanism, leading to differences of up to 10 % in the total emissions. However, the top-down emissions are very sensitive to the bias correction of the observed columns, as the biogenic emissions are 3 times lower when the correction is not applied. Furthermore, the use of different a priori biogenic emissions has a significant impact on the inversion results due to large differences among bottom-up inventories. The sensitivity run using CAMS-GLOB-BIOv3.1 as a priori emissions in the inversion results in 30 % lower emissions with respect to the optimization using MEGAN–MOHYCAN. In regions with large temperature and cloud cover variations, there is strong week-to-week variability in the observed HCHO columns. The top-down emissions, which are optimized at weekly increments, have a much improved capability of representing these large fluctuations than an inversion using monthly increments.</p> |
| first_indexed | 2024-03-08T14:45:29Z |
| format | Article |
| id | doaj.art-e4422cb2d2c94a1d93c0ed8318571ade |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-03-08T14:45:29Z |
| publishDate | 2024-01-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-e4422cb2d2c94a1d93c0ed8318571ade2024-01-11T11:46:19ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242024-01-012444947410.5194/acp-24-449-2024Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021G.-M. Oomen0J.-F. Müller1T. Stavrakou2I. De Smedt3T. Blumenstock4R. Kivi5M. Makarova6M. Palm7A. Röhling8Y. Té9C. Vigouroux10M. M. Friedrich11U. Frieß12F. Hendrick13A. Merlaud14A. Piters15A. Richter16M. Van Roozendael17T. Wagner18Royal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, BelgiumRoyal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, BelgiumRoyal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, BelgiumRoyal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, BelgiumKarlsruhe Institute of Technology (KIT), IMK-ASF, Karlsruhe, GermanyFinnish Meteorological Institute (FMI), Sodankylä, FinlandAtmospheric Physics Department, Saint Petersburg State University, St. Petersburg, RussiaInstitute of Environmental Physics, University of Bremen, Bremen, GermanyKarlsruhe Institute of Technology (KIT), IMK-ASF, Karlsruhe, GermanyLERMA-IPSL, Sorbonne Université, CNRS, Observatoire de Paris, PSL Université, 75005 Paris, FranceRoyal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, BelgiumRoyal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, BelgiumInstitute of Environmental Physics, Heidelberg University, Heidelberg, GermanyRoyal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, BelgiumRoyal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, BelgiumRoyal Netherlands Meteorological Institute (KNMI), De Bilt, the NetherlandsInstitute of Environmental Physics, University of Bremen, Bremen, GermanyRoyal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, BelgiumMax Planck Institute for Chemistry (MPI-C), Mainz, Germany<p>Volatile organic compounds (VOCs) are key precursors of particulate matter and tropospheric ozone. Although the terrestrial biosphere is by far the largest source of VOCs into the atmosphere, the emissions of biogenic VOCs remain poorly constrained at the regional scale. In this work, we derive top-down biogenic emissions over Europe using weekly averaged TROPOMI formaldehyde (HCHO) data from 2018 to 2021. The systematic bias of the TROPOMI HCHO columns is characterized and corrected for based on comparisons with FTIR data at seven European stations. The top-down fluxes of biogenic, pyrogenic, and anthropogenic VOC sources are optimized using an inversion framework based on the MAGRITTEv1.1 chemistry transport model and its adjoint. The inversion leads to strongly increased isoprene emissions with respect to the MEGAN–MOHYCAN inventory over the model domain (from 8.1 to 18.5 <span class="inline-formula">Tg yr<sup>−1</sup></span>), which is driven by the high observed TROPOMI HCHO columns in southern Europe. The impact of the inversion on biomass burning VOCs (<span class="inline-formula">+</span>13 %) and anthropogenic VOCs (<span class="inline-formula">−</span>17 %) is moderate. An evaluation of the optimized HCHO distribution against ground-based remote sensing (FTIR and MAX-DOAS) and in situ data provides generally improved agreement at stations below about 50<span class="inline-formula"><sup>∘</sup></span> N but indicates overestimated emissions in northern Scandinavia. Sensitivity inversions show that the top-down emissions are robust with respect to changes in the inversion settings and in the model chemical mechanism, leading to differences of up to 10 % in the total emissions. However, the top-down emissions are very sensitive to the bias correction of the observed columns, as the biogenic emissions are 3 times lower when the correction is not applied. Furthermore, the use of different a priori biogenic emissions has a significant impact on the inversion results due to large differences among bottom-up inventories. The sensitivity run using CAMS-GLOB-BIOv3.1 as a priori emissions in the inversion results in 30 % lower emissions with respect to the optimization using MEGAN–MOHYCAN. In regions with large temperature and cloud cover variations, there is strong week-to-week variability in the observed HCHO columns. The top-down emissions, which are optimized at weekly increments, have a much improved capability of representing these large fluctuations than an inversion using monthly increments.</p>https://acp.copernicus.org/articles/24/449/2024/acp-24-449-2024.pdf |
| spellingShingle | G.-M. Oomen J.-F. Müller T. Stavrakou I. De Smedt T. Blumenstock R. Kivi M. Makarova M. Palm A. Röhling Y. Té C. Vigouroux M. M. Friedrich U. Frieß F. Hendrick A. Merlaud A. Piters A. Richter M. Van Roozendael T. Wagner Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021 Atmospheric Chemistry and Physics |
| title | Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021 |
| title_full | Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021 |
| title_fullStr | Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021 |
| title_full_unstemmed | Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021 |
| title_short | Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021 |
| title_sort | weekly derived top down volatile organic compound fluxes over europe from tropomi hcho data from 2018 to 2021 |
| url | https://acp.copernicus.org/articles/24/449/2024/acp-24-449-2024.pdf |
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