Preprints
https://doi.org/10.5194/egusphere-2024-1541
https://doi.org/10.5194/egusphere-2024-1541
30 May 2024
 | 30 May 2024
Status: this preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).

Vertical profiles of global tropospheric nitrogen dioxide (NO2) obtained by cloud-slicing TROPOMI

Rebekah P. Horner, Eloise A. Marais, Nana Wei, Robert G. Ryan, and Viral Shah

Abstract. Routine observations of the vertical distribution of tropospheric nitrogen oxides (NOx ≡ NO + NO2) are severely lacking, despite the large influence of NOx on climate, air quality, and atmospheric oxidants. Here we derive vertical profiles of global seasonal mean tropospheric NO2 by applying the cloud-slicing method to TROPOspheric Monitoring Instrument (TROPOMI) columns of NO2 retrieved above optically thick clouds. The resultant NO2 are at a horizontal resolution of 1° × 1° for multiple years (June 2018 to May 2022) covering 5 layers in the upper (180–320 hPa and 320–450 hPa) and mid (450–600 hPa and 600–800 hPa) troposphere, and the marine boundary layer (800 hPa to the Earth’s surface). Terrestrial boundary layer NO2 are obtained as the difference between TROPOMI tropospheric columns and the integrated column of cloud-sliced NO2 in all layers above the boundary layer. Cloud-slicing NO2 is typically 20–60 pptv throughout the free troposphere and spatial coverage ranges from > 60 % in the mid-troposphere to < 20 % in the upper troposphere and boundary layer. Our product is similar (within 10–15 pptv) to NO2 data from NASA DC-8 aircraft campaigns (INTEX-A, ARCTAS, SEAC4RS, ATom) when both datasets are abundant and sampling coverage is commensurate, but such instances are rare. We use the cloud-sliced NO2 to critique current knowledge of the vertical distribution of global NO2, as simulated with the GEOS-Chem chemical transport model updated to include peroxypropionyl nitrate (PPN) and aerosol nitrate photolysis that liberate NO2 in the lower and mid-troposphere for aerosol nitrate photolysis and upper troposphere for PPN. Multiyear GEOS-Chem and cloud-sliced means are compared to mitigate the influence of interannual variability. We find that for cloud-sliced NO2 the interannual variability is ~10 pptv over remote areas and ~25 pptv over areas influenced by lightning and surface sources. The model consistently underestimates NO2 across the remote marine troposphere by ~15 pptv. In the northern midlatitudes, GEOS-Chem overestimates mid-tropospheric NO2 by 20–50 pptv, as NOx production per lightning flash is parameterised to be almost double the rest of the world. There is a critical need for in-situ NO2 measurements in the tropical terrestrial troposphere to evaluate cloud-sliced NO2 there. The model and cloud-sliced NO2 discrepancies identified here need to be investigated further to ensure confident use of models to understand and interpret factors affecting the global distribution of tropospheric NOx, ozone and other oxidants.

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Rebekah P. Horner, Eloise A. Marais, Nana Wei, Robert G. Ryan, and Viral Shah

Status: open (until 12 Jul 2024)

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Rebekah P. Horner, Eloise A. Marais, Nana Wei, Robert G. Ryan, and Viral Shah
Rebekah P. Horner, Eloise A. Marais, Nana Wei, Robert G. Ryan, and Viral Shah

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Short summary
Nitrogen oxides (NOx ≡ NO + NO2) affect tropospheric ozone and the hydroxyl radical, influencing climate and atmospheric oxidation. To address the lack of routine observations of NOx, we cloud-slice satellite observations of NO2 to derive a new dataset of global vertical profiles of NO2. We evaluate our data against in-situ aircraft observations and use our data to critique contemporary knowledge of tropospheric NOx as simulated with the GEOS-Chem model.