Meteorological fields calculated by numerical weather prediction (NWP) models drive offline chemical transport models (CTMs) to solve the transport, chemical reactions, and atmospheric interaction over the geographical domain of interest. HARMONIE (HIRLAM ALADIN Research on Mesoscale Operational NWP in Euromed) is a state-of-The-Art non-hydrostatic NWP community model used at several European weather agencies to forecast weather at the local and/or regional scale. In this work, the HARMONIE WINS50 (cycle 43 cy43) reanalysis dataset at a resolution of 0.025°ĝ€¯×ĝ€¯0.025° covering an area surrounding the North Sea for the years 2019-2021 was coupled offline to the LOTOS-EUROS (LOng-Term Ozone Simulation-EURopean Operational Smog model, v2.2.002) CTM. The impact of using either meteorological fields from HARMONIE or from ECMWF on LOTOS-EUROS simulations of NO2 has been evaluated against ground-level observations and TROPOMI tropospheric NO2 vertical columns. Furthermore, the difference between crucial meteorological input parameters such as the boundary layer height and the vertical diffusion coefficient between the hydrostatic ECMWF and non-hydrostatic HARMONIE data has been studied, and the vertical profiles of temperature, humidity, and wind are evaluated against meteorological observations at Cabauw in The Netherlands. The results of these first evaluations of the LOTOS-EUROS model performance in both configurations are used to investigate current uncertainties in air quality forecasting in relation to driving meteorological parameters and to assess the potential for improvements in forecasting pollution episodes at high resolutions based on the HARMONIE NWP model.

The aim of this paper is to highlight how TROPOspheric Monitoring Instrument (TROPOMI) trace gas data can best be used and interpreted to understand event-based impacts on air quality from regional to city scales around the globe. For this study, we present the observed changes in the atmospheric column amounts of five trace gases (NO2, SO2, CO, HCHO, and CHOCHO) detected by the Sentinel-5P TROPOMI instrument and driven by reductions in anthropogenic emissions due to COVID-19 lockdown measures in 2020. We report clear COVID-19-related decreases in TROPOMI NO2 column amounts on all continents. For megacities, reductions in column amounts of tropospheric NO2 range between 14g % and 63g %. For China and India, supported by NO2 observations, where the primary source of anthropogenic SO2 is coal-fired power generation, we were able to detect sector-specific emission changes using the SO2 data. For HCHO and CHOCHO, we consistently observe anthropogenic changes in 2-week-Averaged column amounts over China and India during the early phases of the lockdown periods. That these variations over such a short timescale are detectable from space is due to the high resolution and improved sensitivity of the TROPOMI instrument. For CO, we observe a small reduction over China, which is in concert with the other trace gas reductions observed during lockdown; however, large interannual differences prevent firm conclusions from being drawn. The joint analysis of COVID-19-lockdown-driven reductions in satellite-observed trace gas column amounts using the latest operational and scientific retrieval techniques for five species concomitantly is unprecedented. However, the meteorologically and seasonally driven variability of the five trace gases does not allow for drawing fully quantitative conclusions on the reduction in anthropogenic emissions based on TROPOMI observations alone. We anticipate that in future the combined use of inverse modeling techniques with the high spatial resolution data from S5P/TROPOMI for all observed trace gases presented here will yield a significantly improved sector-specific, space-based analysis of the impact of COVID-19 lockdown measures as compared to other existing satellite observations. Such analyses will further enhance the scientific impact and societal relevance of the TROPOMI mission.

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.

Nitrogen oxides (NO_x) are air pollutants critical to ozone and fine particle production in the troposphere. Here, we present fuel-based emission inventories updated to 2018, including for mobile source engines using the Fuel-based Inventory of Vehicle Emissions (FIVEs) and oil and gas production using the Fuel-based Oil and Gas (FOG) inventory. The updated FIVE emissions are now consistent with the NEI17 estimates differing within 2% across the contiguous US (CONUS). Tropospheric NO₂ columns modeled by the Weather Research and Forecasting with Chemistry model (WRF-Chem) are compared with those observed by TROPOspheric Monitoring Instrument (TROPOMI) and Ozone Monitoring Instrument (OMI) during the summer of 2018. Modeled NO₂ columns show strong temporal and spatial correlations with TROPOMI (OMI), identified with biases of −3% (−21%) over CONUS, and +8% (−6%) over point sources plus urban regions. Taking account of the negative bias (∼20%) in early version of TROPOMI over polluted regions, WRF-Chem shows good performance with updated FIVE and FOG emissions. Our model tends to under-predict the tropospheric NO₂ columns over background and rural regions (bias of −21% to −3%). Through model sensitivity analyses, we demonstrate the important roles of emissions from soils (11.7% average over CONUS), oil and gas production (4.1%), wildfires (10.6%), and lightning (2.3%) with greater contributions at regional scales. This work provides a roadmap for satellite-based evaluations for emission updates from various sources.

We present a new divergence method to estimated methane (CH₄) emissions from satellite observed mean mixing ratio of methane (XCH₄) by deriving the regional enhancement of XCH₄ in the Planetary Boundary Layer (PBL). The applicability is proven by comparing the estimated emissions with its known emission inventory from a 3-month GEOS-Chem simulation. When applied to TROPOspheric Monitoring Instrument observations, sources from well-known oil/gas production areas, livestock farms and wetlands in Texas become clearly visible in the emission maps. The calculated yearly averaged total CH₄ emission over the Permian Basin is 3.06 (2.82, 3.78) Tg a⁻¹ for 2019, which is consistent with previous studies and double that of EDGAR v4.3.2 for 2012. Sensitivity tests on PBL heights, on the derived regional background and on wind speeds suggest our divergence method is quite robust. It is also a fast and simple method to estimate the CH₄ emissions globally.

The global fire emission inventories depend on ground and airborne measurements of species-specific emission factors (EFs), which translate dry matter losses due to fires to actual trace gas and aerosol emissions. The EFs of nitrogen oxides (NOx) and carbon monoxide (CO) can function as a proxy for combustion efficiency to distinguish flaming from smoldering combustion. The uncertainties in these EFs remain large as they are limited by the spatial and temporal representativeness of the measurements. The global coverage of satellite observations has the advantage of filling this gap, making these measurements highly complementary to ground-based or airborne data. We present a new analysis of biomass burning pollutants using space-borne data to investigate the spatiotemporal efficiency of fire combustion. Column measurements of nitrogen dioxide and carbon monoxide from the TROPOspheric Monitoring Instrument (TROPOMI) are used to quantify the relative atmospheric enhancements of these species over different fire-prone regions around the world. We find spatial and temporal patterns in the classCombining double low linespan classCombining double low lineratio that point to distinct differences in biomass burning behavior. Such differences are induced by the burning phase of the fire (e.g., high-temperature flaming vs. low-temperature smoldering combustion) and burning practice (e.g., the combustion of logs, coarse woody debris and soil organic matter vs. the combustion of fine fuels such as savanna grasses). The sampling techniques and the signal-to-noise ratio of the retrieved <span classCombining double low signals were quantified with WRF-Chem experiments and showed similar distinct differences in combustion types. The TROPOMI measurements show that the fraction of surface smoldering combustion is much larger for the boreal forest fires in the upper Northern Hemisphere and peatland fires in Indonesia. These types of fires cause a much larger increase (3 to 6 times) in <span classCombining double low lineinline-formula relative to span classCombining double low lineinline-formula than elsewhere in the world. The high spatial and temporal resolution of TROPOMI also enables the detection of spatial gradients in combustion efficiency at smaller regional scales. For instance, in the Amazon, we found higher combustion efficiency (up to 3-fold) for savanna fires than for the nearby tropical deforestation fires. Out of two investigated fire emission products, the TROPOMI measurements support the broad spatial pattern of combustion efficiency rooted in GFED4s. Meanwhile, TROPOMI data also add new insights into regional variability in combustion characteristics that are not well represented in the different emission inventories, which can help the fire modeling community to improve their representation of the spatiotemporal variability in EFs.

Airborne and ground-based Pandora spectrometer NOspan classCombining double low line"inline-formula"2/span column measurements were collected during the 2018 Long Island Sound Tropospheric Ozone Study (LISTOS) in the New York City/Long Island Sound region, which coincided with early observations from the Sentinel-5P TROPOspheric Monitoring Instrument (TROPOMI) instrument. Both airborne- and ground-based measurements are used to evaluate the TROPOMI NOspan classCombining double low line"inline-formula"2/span Tropospheric Vertical Column (TrVC) product v1.2 in this region, which has high spatial and temporal heterogeneity in NOspan classCombining double low line"inline-formula"2/span. First, airborne and Pandora TrVCs are compared to evaluate the uncertainty of the airborne TrVC and establish the spatial representativeness of the Pandora observations. The 171 coincidences between Pandora and airborne TrVCs are found to be highly correlated (span classCombining double low line"inline-formula"ir/i2Combining double low line/spanthinsp;0.92 and slope of 1.03), with the largest individual differences being associated with high temporal and/or spatial variability. These reference measurements (Pandora and airborne) are complementary with respect to temporal coverage and spatial representativity. Pandora spectrometers can provide continuous long-term measurements but may lack areal representativity when operated in direct-sun mode. Airborne spectrometers are typically only deployed for short periods of time, but their observations are more spatially representative of the satellite measurements with the added capability of retrieving at subpixel resolutions of 250thinsp;mthinsp;span classCombining double low line"inline-formula"×/spanthinsp;250thinsp;m over the entire TROPOMI pixels they overfly. Thus, airborne data are more correlated with TROPOMI measurements (span classCombining double low line"inline-formula"ir/i2Combining double low line0.96/span) than Pandora measurements are with TROPOMI (span classCombining double low line"inline-formula"ir/i2Combining double low line0.84/span). The largest outliers between TROPOMI and the reference measurements appear to stem from too spatially coarse a priori surface reflectivity (0.5span classCombining double low line"inline-formula"g /span) over bright urban scenes. In this work, this results during cloud-free scenes that, at times, are affected by errors in the TROPOMI cloud pressure retrieval impacting the calculation of tropospheric air mass factors. This factor causes a high bias in TROPOMI TrVCs of 4thinsp;%-11thinsp;%. Excluding these cloud-impacted points, TROPOMI has an overall low bias of 19thinsp;%-33thinsp;% during the LISTOS timeframe of June-September 2018. Part of this low bias is caused by coarse a priori profile input from the TM5-MP model; replacing thesespan idCombining double low line"page6114"/ profiles with those from a 12thinsp;km North American Model-Community Multiscale Air Quality (NAMCMAQ) analysis results in a 12thinsp;%-14thinsp;% increase in the TrVCs. Even with this improvement, the TROPOMI-NAMCMAQ TrVCs have a 7thinsp;%-19thinsp;% low bias, indicating needed improvement in a priori assumptions in the air mass factor calculation. Future work should explore additional impacts of a priori inputs to further assess the remaining low biases in TROPOMI using these datasets./.

Spaceborne NO₂ column observations from two high-resolution instruments, Tropospheric Monitoring Instrument (TROPOMI) on board Sentinel-5 Precursor and Ozone Monitoring Instrument (OMI) on Aura, reveal unprecedented NO₂ decreases over China, South Korea, western Europe, and the United States as a result of public health measures enforced to contain the coronavirus disease outbreak (Covid-19) in January–April 2020. The average NO₂ column drop over all Chinese cities amounts to −40% relative to the same period in 2019 and reaches up to a factor of ~2 at heavily hit cities, for example, Wuhan, Jinan, while the decreases in western Europe and the United States are also significant (−20% to −38%). In contrast with this, although Iran is also strongly affected by the disease, the observations do not show evidence of lower emissions, reflecting more limited health measures.

The Tropospheric Monitoring Instrument (TROPOMI), aboard the Sentinel-5 Precursor (S5P) satellite, launched on 13 October 2017, provides measurements of atmospheric trace gases and of cloud and aerosol properties at an unprecedented spatial resolution of approximately 7 × 3:5 km² (approx. 5:5 × 3:5 km² as of 6 August 2019), achieving near-global coverage in 1 d. The retrieval of nitrogen dioxide (NO₂) concentrations is a three-step procedure: slant column density (SCD) retrieval, separation of the SCD in its stratospheric and tropospheric components, and conversion of these into vertical column densities. This study focusses on the TROPOMI NO₂ SCD retrieval: the retrieval method used, the stability of the SCDs and the SCD uncertainties, and a comparison with the Ozone Monitoring Instrument (OMI) NO₂ SCDs. The statistical uncertainty, based on the spatial variability of the SCDs over a remote Pacific Ocean sector, is 8.63 μmol m^-2 for all pixels (9.45 μmol m^-2 for clear-sky pixels), which is very stable over time and some 30 % less than the long-term average over OMI-QA4ECV data (since the pixel size reduction TROPOMI uncertainties are ~ 8 % larger). The SCD uncertainty reported by the differential optical absorption spectroscopy (DOAS) fit is about 10 % larger than the statistical uncertainty, while for OMI-QA4ECV the DOAS uncertainty is some 20 % larger than its statistical uncertainty. Comparison of the SCDs themselves over the Pacific Ocean, averaged over 1 month, shows that TROPOMI is about 5 % higher than OMI-QA4ECV, which seems to be due mainly to the use of the so-called intensity offset correction in OMI-QA4ECV but not in TROPOMI: turning that correction off means about 5 % higher SCDs. The row-torow variation in the SCDs of TROPOMI, the "stripe amplitude", is 2.15 μmol m, while for OMI-QA4ECV it is a factor of ~ 2 (~ 5) larger in 2005 (2018); still, a so-called stripe correction of this non-physical across-track variation is useful for TROPOMI data. In short, TROPOMI shows a superior performance compared with OMI-QA4ECV and operates as anticipated from instrument specifications. The TROPOMI data used in this study cover 30 April 2018 up to 31 January 2020.

Nitrogen dioxide (NO₂) is a regulated air pollutant that is of particular concern in many cities, where concentrations are high. Emissions of nitrogen oxides to the atmosphere lead to the formation of ozone and particulate matter, with adverse impacts on human health and ecosystems. The effects of emissions are often assessed through modeling based on inventories relying on indirect information that is often outdated or incomplete. Here we show that NO₂ measurements from the new, high-resolution TROPOMI satellite sensor can directly determine the strength and distribution of emissions from Paris. From the observed build-up of NO₂ pollution, we find highest emissions on cold weekdays in February 2018, and lowest emissions on warm weekend days in spring 2018. The new measurements provide information on the spatio-temporal distribution of emissions within a large city, and suggest that Paris emissions in 2018 are only 5–15% below inventory estimates for 2011–2012, reflecting the difficulty of meeting NO_x emission reduction targets.

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.

This overview paper highlights the successes of the Ozone Monitoring Instrument (OMI) on board the Aura satellite spanning a period of nearly 14 years. Data from OMI has been used in a wide range of applications and research resulting in many new findings. Due to its unprecedented spatial resolution, in combination with daily global coverage, OMI plays a unique role in measuring trace gases important for the ozone layer, air quality, and climate change. With the operational very fast delivery (VFD; direct readout) and near real-time (NRT) availability of the data, OMI also plays an important role in the development of operational services in the atmospheric chemistry domain.

Chemical transport models together with emission inventories are widely used to simulate NO2 concentrations over China, but validation of the simulations with in situ measurements has been extremely limited. Here we use ground measurements obtained from the air quality monitoring network recently developed by the Ministry of Environmental Protection of China to validate modeling surface NO2 concentrations from the CHIMERE regional chemical transport model driven by the satellite-derived DECSO and the bottom-up MIX emission inventories. We applied a correction factor to the observations to account for the interferences of other oxidized nitrogen compounds (NOz), based on the modeled ratio of NO2 to NOz. The model accurately reproduces the spatial variability in NO2 from in situ measurements, with a spatial correlation coefficient of over 0.7 for simulations based on both inventories. A negative and positive bias is found for the simulation with the DECSO (slope= 0.74 and 0.64 for the daily mean and daytime only) and the MIX (slope= 1.3 and 1.1) inventories, respectively, suggesting an underestimation and overestimation of NOx emissions from corresponding inventories. The bias between observed and modeled concentrations is reduced, with the slope dropping from 1.3 to 1.0 when the spatial distribution of NOx emissions in the DECSO inventory is applied as the spatial proxy for the MIX inventory, which suggests an improvement of the distribution of emissions between urban and suburban or rural areas in the DECSO inventory compared to that used in the bottom-up inventory. A rough estimate indicates that the observed concentrations, from sites predominantly placed in the populated urban areas, may be 10-40 % higher than the corresponding model grid cell mean. This reduces the estimate of the negative bias of the DECSO-based simulation to the range of -30 to 0 % on average and more firmly establishes that the MIX inventory is biased high over major cities. The performance of the model is comparable over seasons, with a slightly worse spatial correlation in summer due to the difficulties in resolving the more active NOx photochemistry and larger concentration gradients in summer by the model. In addition, the model well captures the daytime diurnal cycle but shows more significant disagreement between simulations and measurements during nighttime, which likely produces a positive model bias of about 15 % in the daily mean concentrations. This is most likely related to the uncertainty in vertical mixing in the model at night.