To new heights by flying low: Comparison of aircraft vertical NO₂ profiles to model simulations and implications for TROPOMI NO₂ retrievals

Abstract

Abstract. The sensitivity of satellites to air pollution close to the sea surface is decreased by scattering of light in the atmosphere and low sea surface albedo. To reliably retrieve tropospheric nitrogen dioxide (NO2) columns using the TROPOspheric Monitoring Instrument (TROPOMI), it is therefore necessary to have good a priori knowledge of the vertical distribution of NO2. In this study, we use an aircraft of the Royal Belgian Institute of Natural Sciences, which was already equipped with a sniffer sensor system, measuring NOx (= NO + NO2), CO2 and SO2. This instrumentation enables us to evaluate vertical profile shapes from several chemical transport models and to validate TROPOMI tropospheric NO2 columns over the polluted North Sea in the summer of 2021.We observe multiple clear signatures of ship plumes from seconds after emission to multiple kilometers downwind. Besides that, our results show that the chemical transport model TM5-MP, which is used in the retrieval of the operational TROPOMI NO2 data, tends to underestimate surface level pollution while overestimating NO2 at higher levels over the study region. The higher horizontal resolution in the regional CAMS ensemble mean and LOTOS-EUROS model improve the surface level pollution estimates, but the models still systematically overestimate NO2 levels at higher altitudes, indicating exaggerated vertical mixing in the models over the North Sea. When replacing the TM5 a priori NO2 profiles with the aircraft-measured NO2 profiles in the air mass factor (AMF) calculation, we find smaller recalculated AMFs. Subsequently, the retrieved NO2 columns increase by 20 %, indicating a significant negative bias in the operational TROPOMI NO2 data product (up to v2.3.1) over the North Sea. This negative bias has important implications for estimating emissions over the sea. While TROPOMI NO2 negative biases caused by the TM5 a priori profiles have also been reported over land, the reduced vertical mixing and smaller surface albedo over sea makes this issue especially relevant over sea and coastal regions.