In this paper, we present the estimation of surface NO2 concentrations over Germany using a machine learning approach. TROPOMI satellite observations of tropospheric NO2 vertical column densities (VCDs) and several meteorological parameters are used to train the neural network model for the prediction of surface NO2 concentrations. The neural network model is validated against ground-based in situ air quality monitoring network measurements and regional chemical transport model (CTM) simulations. Neural network estimation of surface NO2 concentrations show good agreement with in situ monitor data with Pearson correlation coefficient (R) of 0.80. The results also show that the machine learning approach is performing better than regional CTM simulations in predicting surface NO2 concentrations. We also performed a sensitivity analysis for each input parameter of the neural network model. The validated neural network model is then used to estimate surface NO2 concentrations over Germany from 2018 to 2020. Estimated surface NO2 concentrations are used to investigate the spatio-temporal characteristics, such as seasonal and weekly variations of NO2 in Germany. The estimated surface NO2 concentrations provide comprehensive information of NO2 spatial distribution which is very useful for exposure estimation. We estimated the annual average NO2 exposure for 2018, 2019 and 2020 is 15.53, 15.24 and 13.27 µµg/m3, respectively. While the annual average NO2 concentration of 2018, 2019 and 2020 is only 12.79, 12.60 and 11.15 µµg/m3. In addition, we used the surface NO2 data set to investigate the impacts of the coronavirus disease 2019 (COVID-19) pandemic on ambient NO2 levels in Germany. In general, 10–30% lower surface NO2 concentrations are observed in 2020 compared to 2018 and 2019, indicating the significant impacts of a series of restriction measures to reduce the spread of the virus.

Abstract. Launched in October 2017, the TROPOspheric Monitoring Instrument (TROPOMI) aboard Sentinel-5 Precursor provides the potential to monitor air quality over point sources across the globe with a spatial resolution as high as 5.5 km × 3.5 km (7 km × 3.5 km before 6 August 2019). The DLR nitrogen dioxide (NO2) retrieval algorithm for the TROPOMI instrument consists of three steps: the spectral fitting of the slant column, the separation of stratospheric and tropospheric contributions, and the conversion of the slant column to a vertical column using an air mass factor (AMF) calculation. In this work, an improved DLR tropospheric NO2 retrieval algorithm from TROPOMI measurements over Europe is presented. The stratospheric estimation is implemented using the STRatospheric Estimation Algorithm from Mainz (STREAM), which was developed as a verification algorithm for TROPOMI and does not require chemistry transport model data as input. A directionally dependent STREAM (DSTREAM) is developed to correct for the dependency of the stratospheric NO2 on the viewing geometry by up to 2×1014 molec./cm2. Applied to synthetic TROPOMI data, the uncertainty in the stratospheric column is 3.5×1014 molec./cm2 in the case of significant tropospheric sources. Applied to actual measurements, the smooth variation of stratospheric NO2 at low latitudes is conserved, and stronger stratospheric variation at higher latitudes is captured. For AMF calculation, the climatological surface albedo data are replaced by geometry-dependent effective Lambertian equivalent reflectivity (GE_LER) obtained directly from TROPOMI measurements with a high spatial resolution. Mesoscale-resolution a priori NO2 profiles are obtained from the regional POLYPHEMUS/DLR chemistry transport model with the TNO-MACC emission inventory. Based on the latest TROPOMI operational cloud parameters, a more realistic cloud treatment is provided by a Clouds-As-Layers (CAL) model, which treats the clouds as uniform layers of water droplets, instead of the Clouds-As-Reflecting-Boundaries (CRB) model, in which clouds are simplified as Lambertian reflectors. For the error analysis, the tropospheric AMF uncertainty, which is the largest source of NO2 uncertainty for polluted scenarios, ranges between 20 % and 50 %, leading to a total uncertainty in the tropospheric NO2 column in the 30 %–60 % range. From a validation performed with ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements, the new DLR tropospheric NO2 data show good correlations for nine European urban/suburban stations, with an average correlation coefficient of 0.78. The implementation of the algorithm improvements leads to a decrease of the relative difference from −55.3 % to −34.7 % on average in comparison with the DLR reference retrieval. When the satellite averaging kernels are used to remove the contribution of a priori profile shape, the relative difference decreases further to ∼ −20 %.

Abstract. Launched in October 2017, the TROPOspheric Monitoring Instrument (TROPOMI) aboard Sentinel-5 Precursor provides the potential to monitor air quality over point sources across the globe with a spatial resolution as high as 5.5 km × 3.5 km (7 km × 3.5 km before 6 August 2019). The nitrogen dioxide (NO2) retrieval algorithm for the TROPOMI instrument consists of three steps: the spectral fitting of the slant column, the separation of stratospheric and tropospheric contributions, and the conversion of the slant column to a vertical column using an air mass factor (AMF) calculation. In this work, an improved tropospheric NO2 retrieval algorithm from TROPOMI measurements over Europe is presented. The stratospheric estimation is implemented using the STRatospheric Estimation Algorithm from Mainz (STREAM), which was developed as a verification algorithm for TROPOMI and does not require chemistry transport model data as input. A directionally dependent STREAM (DSTREAM) is developed to correct for the dependency of the stratospheric NO2 on the viewing geometry by up to 2 × 1014 molec/cm2. Applied to synthetic TROPOMI data, the uncertainty in the stratospheric column is 3.5 × 1014 molec/cm2 for polluted conditions. Applied to actual measurements, the smooth variation of stratospheric NO2 at low latitudes is conserved, and stronger stratospheric variation at higher latitudes are captured. For AMF calculation, the climatological surface albedo data is replaced by geometry-dependent effective Lambertian equivalent reflectivity (GE_LER) obtained directly from TROPOMI measurements with a high spatial resolution. Mesoscale-resolution a priori NO2 profiles are obtained from the regional POLYPHEMUS/DLR chemistry transport model with the TNO-MACC emission inventory. Based on the latest TROPOMI operational cloud parameters, a more realistic cloud treatment is provided by a clouds-as-layers (CAL) model, which treats the clouds as uniform layers of water droplets, instead of the clouds-as-reflecting-boundaries (CRB) model, in which clouds are simplified as Lambertian reflectors. For the error analysis, the tropospheric AMF uncertainty, which is the largest source of NO2 uncertainty for polluted scenarios, ranges between 20 % and 50 %, leading to a total uncertainty in the tropospheric NO2 column in the 30–60 % range. From a validation performed with ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements, the improved tropospheric NO2 data shows good correlations for nine European urban/suburban stations with an average correlation coefficient of 0.78. The implementation of the algorithm improvements leads to a decrease of the relative difference from −55.3 % to −34.7 % on average.

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Chemical-transport models are a persuasive tool to predict and study air pollution on different temporal and spatial scales. However, due to the complexity of physics and chemistry of air pollutants' interactions and lack of precise input data, these models have uncertainties. In particular, most of the emission data have a too coarse resolution and are not appropriate for application in urban scale air quality modeling. In this study, a downscaling approach is utilized for emission data in order to improve the air pollutants concentration simulation over Munich city using the POLYPHEMUS/DLR chemistry-transport model (CTM). Traffic emission from the Bavarian Emission Kataster (EKATBY) 2004 anthropogenic emissions dataset with 2 km resolution is downscaled to 100 m with regard to the highresolution OpenStreetMap roads paths and areal emission sources are relocated on the most populated and active sites which have been determined from VIIRS NOAA satellite-derived night light data. In addition, the EEA CORINE 2012 land use data is implemented with 100 m grid resolution to improve e.g. the biogenic emissions. Regarding aerosols, the SIze REsolved Aerosol Module (SIREAM) for aerosol dynamic and the Secondary Organic Aerosol Model (SORGAM) are applied. The CTM is driven by WRF 3.5 meteorological forecasts. In order to have reliable simulations, the one-way grid nesting method with four domains is employed, where the coarsest domain covers Europe and the finest covers Munich city area.