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

<p>The sensitivity of satellites to air pollution close to the sea surface is decreased by the scattering of light in the atmosphere and low sea surface albedo. To reliably retrieve tropospheric nitrogen dioxide (NO<span class="inline-formula">₂</span>) columns using the TROPOspheric Monitoring Instrument (TROPOMI), it is therefore necessary to have good a priori knowledge of the vertical distribution of NO<span class="inline-formula">₂</span>. In this study, we use an aircraft of the Royal Belgian Institute of Natural Sciences equipped with a sniffer sensor system to measure NO<span class="inline-formula">_<i>x</i></span> (<span class="inline-formula">=</span> NO <span class="inline-formula">+</span> NO<span class="inline-formula">₂</span>), CO<span class="inline-formula">₂</span> and SO<span class="inline-formula">₂</span>. This instrumentation enabled us to evaluate vertical profile shapes from several chemical transport models and to validate TROPOMI tropospheric NO<span class="inline-formula">₂</span> columns over the polluted North Sea in the summer of 2021. The aircraft sensor observes multiple clear signatures of ship plumes from seconds after emission to multiple kilometers downwind. Besides that, our results show that the chemical transport model Transport Model 5, Massively Parallel version (TM5-MP), which is used in the retrieval of the operational TROPOMI NO<span class="inline-formula">₂</span> data, tends to underestimate surface level pollution – especially under conditions without land outflow – while overestimating NO<span class="inline-formula">₂</span> at higher levels over the study region. The higher horizontal resolution in the regional CAMS (Copernicus Atmosphere Monitoring Service) ensemble mean and the LOTOS-EUROS (Long Term Ozone Simulation European Operational Smog) model improves the surface level pollution estimates. However, the models still systematically overestimate NO<span class="inline-formula">₂</span> levels at higher altitudes, indicating exaggerated vertical mixing and overall too much NO<span class="inline-formula">₂</span> in the models over the North Sea. When replacing the TM5 a priori NO<span class="inline-formula">₂</span> profiles with the aircraft-measured NO<span class="inline-formula">₂</span> profiles in the air mass factor (AMF) calculation, we find smaller recalculated AMFs. Subsequently, the retrieved NO<span class="inline-formula">₂</span> columns increase by 20 %, indicating a significant negative bias in the operational TROPOMI NO<span class="inline-formula">₂</span> 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 NO<span class="inline-formula">₂</span> 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 make this issue especially relevant over sea and coastal regions.</p>