Nitrogen dioxide (NO2) is one of the main data products measured by the Tropospheric Monitoring Instrument (TROPOMI) on the Sentinel-5 Precursor (S5P) satellite, which combines a high signal-to-noise ratio with daily global coverage and high spatial resolution. TROPOMI provides a valuable source of information to monitor emissions from local sources such as power plants, industry, cities, traffic and ships, and variability of these sources in time. Validation exercises of NO2 v1.2-v1.3 data, however, have revealed that TROPOMI's tropospheric vertical column densities (VCDs) are too low by up to 50ĝ€¯% over highly polluted areas. These findings are mainly attributed to biases in the cloud pressure retrieval, the surface albedo climatology and the low resolution of the a priori profiles derived from global simulations of the TM5-MP chemistry model. This study describes improvements in the TROPOMI NO2 retrieval leading to version v2.2, operational since 1 July 2021. Compared to v1.x, the main changes are the following. (1) The NO2-v2.2 data are based on version-2 level-1b (ir)radiance spectra with improved calibration, which results in a small and fairly homogeneous increase in the NO2 slant columns of 3% to 4%, most of which ends up as a small increase in the stratospheric columns. (2) The cloud pressures are derived with a new version of the FRESCO cloud retrieval already introduced in NO2-v1.4, which led to a lowering of the cloud pressure, resulting in larger tropospheric NO2 columns over polluted scenes with a small but non-zero cloud coverage. (3) For cloud-free scenes a surface albedo correction is introduced based on the observed reflectance, which also leads to a general increase in the tropospheric NO2 columns over polluted scenes of order 15%. (4) An outlier removal was implemented in the spectral fit, which increases the number of good-quality retrievals over the South Atlantic Anomaly region and over bright clouds where saturation may occur. (5) Snow/ice information is now obtained from ECMWF weather data, increasing the number of valid retrievals at high latitudes. On average the NO2-v2.2 data have tropospheric VCDs that are between 10% and 40% larger than the v1.x data, depending on the level of pollution and season; the largest impact is found at mid and high latitudes in wintertime. This has brought these tropospheric NO2 closer to Ozone Monitoring Instrument (OMI) observations. Ground-based validation shows on average an improvement of the negative bias of the stratospheric (from-6% to-3%), tropospheric (from-32% to-23%) and total (from-12% to-5%) columns. For individual measurement stations, however, the picture is more complex, in particular for the tropospheric and total columns.

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This paper reports on consolidated ground-based validation results of the atmospheric NO2 data produced operationally since April 2018 by the TROPOspheric Monitoring Instrument (TROPOMI) on board of the ESA/EU Copernicus Sentinel-5 Precursor (S5P) satellite. Tropospheric, stratospheric, and total NO2 column data from S5P are compared to correlative measurements collected from, respectively, 19 Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS), 26 Network for the Detection of Atmospheric Composition Change (NDACC) Zenith-Scattered-Light DOAS (ZSL-DOAS), and 25 Pandonia Global Network (PGN)/Pandora instruments distributed globally. The validation methodology gives special care to minimizing mismatch errors due to imperfect spatiotemporal co-location of the satellite and correlative data, e.g. by using tailored observation operators to account for differences in smoothing and in sampling of atmospheric structures and variability and photochemical modelling to reduce diurnal cycle effects. Compared to the ground-based measurements, S5P data show, on average, (i) a negative bias for the tropospheric column data, of typically-23 % to-37 % in clean to slightly polluted conditions but reaching values as high as-51 % over highly polluted areas; (ii) a slight negative median difference for the stratospheric column data, of about-0:2 Pmolec cm-2, i.e. approx.-2 % in summer to-15 % in winter; and (iii) a bias ranging from zero to-50 % for the total column data, found to depend on the amplitude of the total NO2 column, with small to slightly positive bias values for columns below 6 Pmolec cm-2 and negative values above. The dispersion between S5P and correlative measurements contains mostly random components, which remain within mission requirements for the stratospheric column data (0.5 Pmolec cm-2) but exceed those for the tropospheric column data (0.7 Pmolec cm-2). While a part of the biases and dispersion may be due to representativeness differences such as different area averaging and measurement times, it is known that errors in the S5P tropospheric columns exist due to shortcomings in the (horizontally coarse) a priori profile representation in the TM5-MP chemical transport model used in the S5P retrieval and, to a lesser extent, to the treatment of cloud effects and aerosols. Although considerable differences (up to 2 Pmolec cm-2 and more) are observed at single ground-pixel level, the near-real-time (NRTI) and offline (OFFL) versions of the S5P NO2 operational data processor provide similar NO2 column values and validation results when globally averaged, with the NRTI values being on average 0.79 % larger than the OFFL values. @en

Satellite retrieval of vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO₂) is critical for NO_x pollution and impact evaluation. For regions with high aerosol loadings, the retrieval accuracy is greatly affected by whether aerosol optical effects are treated implicitly (as additional effective clouds) or explicitly, among other factors. Our previous POMINO algorithm explicitly accounts for aerosol effects to improve the retrieval, especially in polluted situations over China, by using aerosol information from GEOS-Chem simulations with further monthly constraints by MODIS/Aqua aerosol optical depth (AOD) data. Here we present a major algorithm update, POMINO v1.1, by constructing a monthly climatological dataset of aerosol extinction profiles, based on level 2 CALIOP/CALIPSO data over 2007-2015, to better constrain the modeled aerosol vertical profiles. We find that GEOS-Chem captures the month-to-month variation in CALIOP aerosol layer height (ALH) but with a systematic underestimate by about 300-600 m (season and location dependent), due to a too strong negative vertical gradient of extinction above 1 km. Correcting the model aerosol extinction profiles results in small changes in retrieved cloud fraction, increases in cloud-top pressure (within 2 %-6 % in most cases), and increases in tropospheric NO₂ VCD by 4 %-16 % over China on a monthly basis in 2012. The improved NO₂ VCDs (in POMINO v1.1) are more consistent with independent ground-based MAX-DOAS observations (R²=0.80, NMB =-3.4 %, for 162 pixels in 49 days) than POMINO (R²=0.80, NMB =-9.6 %), DOMINO v2 (R²=0.68, NMB =-2.1 %), and QA4ECV (R²=0.75, NMB =-22.0 %) are. Especially on haze days, R² reaches 0.76 for POMINO v1.1, much higher than that for POMINO (0.68), DOMINO v2 (0.38), and QA4ECV (0.34). Furthermore, the increase in cloud pressure likely reveals a more realistic vertical relationship between cloud and aerosol layers, with aerosols situated above the clouds in certain months span id=page2 instead of always below the clouds. The POMINO v1.1 algorithm is a core step towards our next public release of the data product (POMINO v2), and it will also be applied to the recently launched S5P-TROPOMI sensor.

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