Preprints
https://doi.org/10.5194/egusphere-2024-2912
https://doi.org/10.5194/egusphere-2024-2912
27 Sep 2024
 | 27 Sep 2024
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model

Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther

Abstract. Natural emissions (vegetation, soil, lightning) are the dominant sources of non-methane biogenic volatile organic compounds (BVOCs) and nitrogen oxides (NOx ≡ NO + NO2) released into the atmosphere over Africa. BVOCs and NOx interact with each other and strongly impact their own chemical lifetimes and degradation pathways, in particular through their influence on hydroxyl radical levels. To account for this intricate interplay between NOx and VOCs, we design and apply a novel inversion setup aiming at the simultaneous optimisation of monthly VOC and NOx emissions in 2019 in a regional chemistry-transport model, based on TROPOMI HCHO and NO2 satellite observations. The TROPOMI-based inversions suggest substantial underestimations of natural NOx and VOC emissions used as a priori in the model. The annual flux over Africa is increased from 125 to 165 Tg yr−1 for isoprene, and from 1.9 to 2.4 TgN yr−1 and from 0.5 to 2.0 TgN yr−1 for the soil and lightning NO emissions, respectively. Despite the NOx emission increase, evaluation against in situ NO2 measurements at seven rural sites in Western Africa displays significant model underestimations after optimisation. The large increases in lightning emissions are supported by comparisons with TROPOMI cloud-sliced upper-tropospheric NO2 volume mixing ratios, which even remain underestimated by the model after optimisation. Our study strongly supports the application of a bias correction to the TROPOMI HCHO data and the use of a double-species constraint (vs single-species inversion), based on comparisons with isoprene columns retrieved from the Cross-track Infrared Sensor (CrIS). 

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Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther

Status: open (until 08 Nov 2024)

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Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther

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Short summary
Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimise these natural emissions over Africa in 2019. Our approach led to an increase in natural emissions that is supported by independent data showing that current estimates are underestimated.