Preprints
https://doi.org/10.5194/egusphere-2023-2456
https://doi.org/10.5194/egusphere-2023-2456
06 Nov 2023
 | 06 Nov 2023
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

Bias characterization of OMI HCHO columns based on FTIR and aircraft measurements and impact on top-down emission estimates

Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried

Abstract. Spaceborne formaldehyde (HCHO) measurements constitute an excellent proxy for the sources of non-methane volatile organic compounds (NMVOCs). Past studies suggested substantial overestimation of NMVOC emissions in state-of-the-art inventories over major source regions. Here, the QA4ECV (Quality Assurance for Essential Climate Variables) retrieval of HCHO columns from OMI (Ozone Monitoring Instrument) are evaluated against (1) FTIR (Fourier-transform infrared) column observations at 26 stations worldwide, and (2) aircraft in situ HCHO measurements from campaigns conducted over the U.S. in 2012–2013. Both validation exercises show that OMI underestimates high columns and overestimates low columns. The linear regression of OMI and aircraft-based columns gives ΩOMI = 0.651 Ωairc + 2.95×1015 molec.cm-2, with ΩOMI and Ωairc the OMI and aircraft-derived vertical columns, whereas the regression of OMI and FTIR data givesΩOMI = 0.659 ΩFTIR + 2.02×1015 molec.cm-2. Inverse modelling of NMVOC emissions with a global model based on OMI columns corrected for biases based on those relationships leads to much-improved agreement against FTIR data and HCHO concentrations from 11 aircraft campaigns. The optimized global isoprene emissions (~445 Tg yr-1) are 25 % higher than those obtained without bias correction. The optimized isoprene emissions bear both striking similarities and differences with recently published emissions based on spaceborne isoprene columns from the CrIS (Cross-track Infrared Sounder) sensor. Although the interannual variability of OMI HCHO columns is well understood over regions where biogenic emissions are dominant, and the HCHO trends over China and India clearly reflect anthropogenic emission changes, the observed HCHO decline over Southeastern U.S. remains imperfectly elucidated.

Jean-François Müller et al.

Status: open (until 18 Dec 2023)

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Jean-François Müller et al.

Jean-François Müller et al.

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Short summary
Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.