NO2 Vertical Column Research Articles

Interpreting summertime hourly variation of NO2 columns with implications for geostationary satellite applications

Abstract. Accurate representation of the hourly variation in the NO2-column-to-surface relationship is essential for interpreting geostationary observations of NO2 columns. Previous research indicated inconsistencies in this hourly variation. This study employs the high-performance configuration of the GEOS-Chem model (GCHP) to analyze daytime hourly NO2 total columns and surface concentrations during summer. We use measurements from globally distributed Pandora sun photometers and aircraft observations over the United States. We correct Pandora total NO2 vertical columns for (1) hourly variations in effective temperature driven by vertically resolved contributions to the total column and (2) changes in local solar time along the Pandora line of sight. These corrections increase the total NO2 columns by 5–6 × 1014 molec. cm−2 at 09:00 and 18:00 across all sites. Fine-scale simulations from GHCP (∼12 km) reduce the normalized bias (NB) against Pandora total NO2 columns from 19 % to 10 % and against aircraft measurements from 25 % to 13 % in Maryland, Texas, and Colorado. Similar reductions are observed in NO2 columns over the eastern US (17 % to 9 %), the western US (22 % to 14 %), Europe (24 % to 15 %), and Asia (29 % to 21 %) when compared to 55 km simulations. Our analysis attributes the weaker hourly variability in the total NO2 column to (1) hourly variations in column effective temperature, (2) local solar time changes along the Pandora line of sight, and (3) differences in hourly NO2 variability from different atmospheric layers, with the lowest 500 m exhibiting greater variability, while the dominant residual column above 500 m exhibits weaker variability.

NitroNet – a machine learning model for the prediction of tropospheric NO2 profiles from TROPOMI observations

Abstract. We introduce NitroNet, a deep learning model for the prediction of tropospheric NO2 profiles from satellite column measurements. NitroNet is a neural network trained on synthetic NO2 profiles from the regional chemistry and transport model WRF-Chem, which was operated on a European domain for the month of May 2019. This WRF-Chem simulation was constrained by in situ and satellite measurements, which were used to optimize important simulation parameters (e.g. the boundary layer scheme). The NitroNet model receives NO2 vertical column densities (VCDs) from the TROPOspheric Monitoring Instrument (TROPOMI) and ancillary variables (meteorology, emissions, etc.) as input, from which it reproduces NO2 concentration profiles. Training of the neural network is conducted on a filtered dataset, meaning that NO2 profiles showing strong disagreement (>20 %) with colocated TROPOMI column measurements are discarded. We present a first evaluation of NitroNet over a variety of geographical and temporal domains (Europe, the US West Coast, India, and China) and different seasons. For this purpose, we validate the NO2 profiles predicted by NitroNet against satellite, in situ, and MAX-DOAS (Multi-Axis Differential Optical Absorption Spectroscopy) measurements. The training data were previously validated against the same datasets. During summertime, NitroNet shows small biases and strong correlations with all three datasets: a bias of +6.7 % and R=0.95 for TROPOMI NO2 VCDs, a bias of −10.5 % and R=0.75 for AirBase surface concentrations, and a bias of −34.3 % to +99.6 % with R=0.83–0.99 for MAX-DOAS measurements. In comparison to TROPOMI satellite data, NitroNet even shows significantly lower errors and stronger correlation than a direct comparison with WRF-Chem numerical results. During wintertime considerable low biases arise because the summertime/late-spring training data are not fully representative of all atmospheric wintertime characteristics (e.g. longer NO2 lifetimes). Nonetheless, the wintertime performance of NitroNet is surprisingly good and comparable to that of classic regional chemistry and transport models. NitroNet can demonstrably be used outside the geographic and temporal domain of the training data with only slight performance reductions. What makes NitroNet unique when compared to similar existing deep learning models is the inclusion of synthetic model data, which offers important benefits: due to the lack of NO2 profile measurements, models trained on empirical datasets are limited to the prediction of surface concentrations learned from in situ measurements. NitroNet, however, can predict full tropospheric NO2 profiles. Furthermore, in situ measurements of NO2 are known to suffer from biases, often larger than +20 %, due to cross-sensitivities to photooxidants, which other models trained on empirical data inevitably reproduce.

Spatiotemporal estimation of surface NO2 concentrations in the Pearl River Delta region based on TROPOMI data and machine learning

Nitrogen dioxide (NO2) is a major air pollutant, and its concentration data are crucial for the study of air pollution and its impact on the environment. Although satellite data provide an effective method for estimating surface concentrations on a large scale through integrated modeling, the estimation of surface NO2 concentrations is hampered by the substantial amount of missing satellite data. This restricts in-depth studies of surface NO2 pollution. This study aims to reconstruct the missing data on tropospheric NO2 vertical column density from the TROPOspheric Monitoring Instrument (TROPOMI NO2). Subsequently, the reconstructed TROPOMI NO2 data and other predictor variables were utilized to estimate the daily surface NO2 concentrations at a 1 km resolution for the Pearl River Delta (PRD) region. The TROPOMI NO2 reconstruction models and the surface NO2 estimation model were both developed using the XGBoost algorithm. Additionally, comparative experiments were conducted between the XGBoost model and other traditional machine learning models, and the performances of the XGBoost model were evaluated through 10-fold cross-validation (CV) sample-based and site-based evaluations. The results indicate that the sample-based and site-based CV R2 values were 0.873 and 0.709, respectively. The feature importance scores indicate that TROPOMI NO2 was the most significant variable contributing to the estimation model. This indicates that the reconstruction of TROPOMI NO2 data and the development of an Extreme Gradient Boosting (XGBoost) model are suitable for the spatiotemporal estimation of surface NO2 concentrations in the PRD region, effectively reflecting the spatiotemporal distribution and evolution of surface NO2 concentrations in the area.

Validation of GEMS tropospheric NO2 columns and their diurnal variation with ground-based DOAS measurements

Abstract. Instruments for air quality observations on geostationary satellites provide multiple observations per day and allow for the analysis of the diurnal variation in important air pollutants such as nitrogen dioxide (NO2). The South Korean instrument GEMS (Geostationary Environmental Monitoring Spectrometer), launched in February 2020, is the first geostationary instrument that is able to observe the diurnal variation in NO2. The measurements have a spatial resolution of 3.5 km × 8 km and cover a large part of Asia. This study compares 1 year of tropospheric NO2 vertical column density (VCD) observations from the operational GEMS L2 product, the scientific GEMS IUP-UB (Institute of Environmental Physics at the University of Bremen) product, the operational TROPOspheric Monitoring Instrument (TROPOMI) product, and ground-based differential optical absorption spectroscopy (DOAS) measurements in South Korea. The GEMS L2 tropospheric NO2 VCDs overestimate the ground-based tropospheric NO2 VCDs with a median relative difference of +61 % and a correlation coefficient of 0.76. The median relative difference is −2 % for the GEMS IUP-UB product and −16 % for the TROPOMI product, with correlation coefficients of 0.83 and 0.89, respectively. The scatter in the GEMS products can be reduced when observations are limited to the TROPOMI overpass time. Diurnal variations in tropospheric NO2 VCDs differ by the pollution level of the analyzed site but with good agreement between the GEMS IUP-UB and ground-based observations. Low-pollution sites show weak or almost no diurnal variation. In summer, the polluted sites show a minimum around noon, indicating the large influence of photochemical loss. Most variation is seen in spring and autumn, with increasing NO2 in the morning, a maximum close to noon, and a decrease towards the afternoon. Winter observations show rather flat or slightly decreasing NO2 throughout the day. Winter observations under low-wind-speed conditions at high-pollution sites show enhancements of NO2 throughout the day. This indicates that under calm conditions, dilution and the less effective chemical loss in winter do not balance the accumulating emissions. Diurnal variation observed at a low-pollution site follows seasonal wind patterns. A weekday–weekend effect analysis shows good agreement between the different products. However, the GEMS L2 product, while agreeing with the other data sets on weekdays, shows significantly less reduction on weekends. The influence of the stratospheric contribution and the surface reflectivity product on the satellite tropospheric NO2 VCD products is investigated. While the TM5 model's stratospheric VCDs, used in the TROPOMI product, are too high, resulting in tropospheric NO2 VCDs that are too low and even negative, when used in the GEMS IUP-UB retrieval, the GEMS L2 stratospheric VCD is too low. Surface reflectivity comparisons indicate that the GEMS L2 reflectivity makes a large contribution to the observed overestimation and scatter.

Tropospheric NO2 retrieval algorithm for geostationary satellite instruments: applications to GEMS

Abstract. In this study, we develop an advanced retrieval algorithm for tropospheric nitrogen dioxide (NO2) from the geostationary satellite instruments and apply it to Geostationary Environment Monitoring Spectrometer (GEMS) observations. Overall, the algorithm follows previous heritage for the polar-orbiting satellites Global Ozone Monitoring Experiment-2 (GOME-2) and Tropospheric Monitoring Instrument (TROPOMI), but several improvements are implemented to account for specific features of geostationary satellites. The DLR GEMS NO2 retrieval employs an extended fitting window compared to the current fitting window used in GEMS operational v2.0 NO2 retrieval, which results in improved spectral fit quality and lower uncertainties. For the stratosphere–troposphere separation in GEMS measurements, two methods are developed and evaluated: (1) STRatospheric Estimation Algorithm from Mainz (STREAM) as used in the DLR TROPOMI NO2 retrieval and adapted to GEMS and (2) estimation of stratospheric NO2 columns from the Copernicus Atmosphere Monitoring Service (CAMS) Integrated Forecast System (IFS) cycle 48R1 model data, which introduce full stratospheric chemistry as it will be used in the operational Sentinel-4 NO2 retrieval. While STREAM provides hourly estimates of stratospheric NO2, it has limitations in describing small-scale variations and exhibits systematic biases near the boundary of the field of view. In this respect, the use of estimated stratospheric NO2 columns from the CAMS forecast model profile demonstrates better applicability by describing not only diurnal variation but also small-scale variations. For the improved air mass factor (AMF) calculation, sensitivity tests are performed using different input data. In our algorithm, cloud fractions retrieved from the Optical Cloud Recognition Algorithm (OCRA) adapted to GEMS level 1 data are applied instead of the GEMS v2.0 cloud fraction. OCRA is used operationally in TROPOMI and Sentinel-4. Compared to the GEMS level 2 cloud fraction which is typically set to around 0.1 for clear-sky scenes, OCRA sets cloud fractions close to or at 0. The OCRA-based cloud corrections result in increased tropospheric AMFs and decreased tropospheric NO2 vertical columns, leading to better agreement with results from existing TROPOMI observations. The effects of surface albedo on GEMS tropospheric NO2 retrievals are assessed by comparing the GEMS v2.0 background surface reflectance (BSR) and TROPOMI Lambertian-equivalent reflectivity (LER) climatology v2.0 product. The differences between the two surface albedo products and their impact on tropospheric AMF are particularly pronounced over snow/ice scenes during winter. A priori NO2 profiles from the CAMS forecast model, applied in the DLR GEMS algorithm, effectively capture variations in NO2 concentrations throughout the day with high spatial resolution and the advanced chemical mechanism, which demonstrates its suitability for geostationary satellite measurements. The retrieved DLR GEMS tropospheric NO2 columns show good capability for capturing hotspot signals at the scale of city clusters and describe spatial gradients from city centres to surrounding areas. Diurnal variations of tropospheric NO2 columns over Asia are well described through hourly sampling of GEMS. Evaluation of DLR GEMS tropospheric NO2 columns against TROPOMI v2.4 and GEMS v2.0 operational products shows overall good agreement. The uncertainty of DLR GEMS tropospheric NO2 vertical columns varies based on observation scenarios. In regions with low pollution levels such as open-ocean and remote rural areas, retrieval uncertainties typically range from 10 % to 50 %, primarily due to uncertainties in slant columns. For heavily polluted regions, uncertainties in tropospheric NO2 columns are mainly driven by errors in tropospheric AMF calculations. Notably, the total uncertainty in GEMS tropospheric NO2 columns is most significant in winter, particularly over heavily polluted regions with low-level clouds below or near the NO2 peak.

Maritime sector contributions on NO2 surface concentrations in major ports of the Mediterranean Basin

The aim of this study is to estimate the contribution of the maritime sector on the air quality of major Mediterranean ports with the Long Term Ozone Simulation-European Operational Smog (LOTOS-EUROS) chemical transport model, using two source apportionment methods: the brute-force emission scenario methodology and the labelling approach. With the brute-force method NO2 shipping concentrations are estimated by the ratio of the difference between two model runs - with original and reduced emissions - and the equivalent emission reduction factor. In the labelling, emitted species are explicitly labelled per sector and tracked through all model processes. Simulations are performed for a one-year period, from May 2018 to May 2019 and the two methodologies are intercompared. The methods show strong agreement between NO2 shipping contributions (R > 0.95) and differences of ∼14%. A sensitivity analysis carried out using the brute-force method indicates that a linear regime between NOX emissions and NO2 concentrations holds, when adopting a low to moderate emission reduction (<50%). We applied the brute-force method with an assumed 20% emission reduction and found that the NO2 surface concentrations attributed to maritime sector activities in selected ports were between 5% and 70% of the total NO2 surface concentrations, with a mean value of 27%. Comparisons between measurements from the European Environment Agency (EEA) ground-based monitoring stations and LOTOS-EUROS NO2 surface concentrations show a strong correlation (R∼0.8) with an underestimation of the model (∼-32%) for the whole period. The bias is reduced to −20% when air quality monitoring stations affected by traffic and industrial activities are excluded from the analysis. Moreover, observed Sentinel-5 Precursor TroPospheric MOnitoring Instrument (S5P/TROPOMI) and modelled NO2 vertical column densities (VCDs) show a significant spatial agreement (R∼0.86) for both summer and winter with biases of −25% and −1%, respectively, over the selected ports. These comparisons were carried out as an indirect way of validating the applied methodology and the performance of the model in coastal areas. The present study provides a solid background which will enable the assimilation of the satellite observations to the CTM to infer NOX shipping emissions in the Mediterranean Basin in view of the upcoming designation of the Mediterranean Sea as an Emission Control Area in 2025.

Investigating the impact of coupling HARMONIE-WINS50 (cy43) meteorology to LOTOS-EUROS (v2.2.002) on a simulation of NO2 concentrations over the Netherlands

Abstract. 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° × 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.

Revised estimates of NO2 reductions during the COVID-19 lockdowns using updated TROPOMI NO2 retrievals and model simulations

The TROPOspheric Monitoring Instrument (TROPOMI) observed unprecedented declines in NO2 vertical column densities (VCD) over the world's most densely populated cities during the 2020 COVID-19 lockdowns. These favorable changes in NO2 air quality were correlated with sharp reductions in traffic volume and economic activity during the lockdowns. In this comprehensive global study, we provide revised estimates of the declines in anthropogenic emissions for 36 megacities using a novel methodology for disentangling the anthropogenic emissions from the meteorological transport and natural variability. We further quantify the uncertainty associated with changes in the a priori profile shape information during the lockdowns due to reduced emissions. Satellite NO2 retrieval techniques calculate an air mass factor that requires a priori NO2 profile shape information representative of the local atmosphere. This information, which is typically obtained from a chemical transport model (CTM), was not available for the early studies. This study also accounts for the satellite sampling errors resulting from the selective sampling of non-cloudy scenes during the study period. For our analysis, we used CTM simulations that were generated with and without COVID-impacted emissions. We perform retrievals of tropospheric NO2 columns with the NASA NO2 algorithm, and then use observed and simulated data to disentangle the meteorological transport from the contribution due anthropogenic emissions. We found that the meteorological transport was most significant source of variability ranging between −35% and 22% of the change total tropospheric VCD. We also find that not accounting for changes in the a priori NO2 profile shape information during the lockdowns resulted in systematic retrieval errors that were up to 12% of the estimated decline, and the elimination of cloud contaminated scenes resulted in sampling errors that in general ranged between varied ±15%.

Evaluation of the first year of Pandora NO2 measurements over Beijing and application to satellite validation

Abstract. Nitrogen dioxide (NO2) is a highly photochemically reactive gas, has a lifetime of only a few hours, and at high concentrations is harmful to human beings. Therefore, it is important to monitor NO2 with high-precision, time-resolved instruments. To this end, a Pandora spectrometer has been installed on the roof of the laboratory building of the Aerospace Information Research Institute of the Chinese Academy of Sciences in the Olympic Park, Beijing, China. The concentrations of trace gases (including NO2, HCHO, O3) measured with Pandora are made available through the open-access Pandora database (https://data.pandonia-global-network.org/Beijing-RADI/Pandora171s1/, last access: 11 July 2023). In this paper, an overview is presented of the Pandora total and tropospheric NO2 vertical column densities (VCDs) and surface concentrations collected during the first year of operation, i.e., from August 2021 to July 2022. The data show that NO2 concentrations were high in the winter and low in the summer, with a diurnal cycle where the concentrations reached a minimum during the daytime. The concentrations were significantly lower during the 2022 Winter Olympics in Beijing, showing the effectiveness of the emission control measures during that period. The Pandora observations show that during northerly winds, clean air is transported to Beijing with low NO2 concentrations, whereas during southerly winds, pollution from surrounding areas is transported to Beijing and NO2 concentrations are high. The contribution of tropospheric NO2 to the total NO2 VCD varies significantly on daily to seasonal timescales; i.e., monthly averages vary between 50 % and 60 % in the winter and between 60 % and 70 % in the spring and autumn. A comparison of Pandora-measured surface concentrations with collocated in situ measurements using a Thermo Scientific 42i-TL analyzer shows that the Pandora data are low and that the relationship between Pandora-derived surface concentrations and in situ measurements is different for low and high NO2 concentrations. Explanations for these differences are offered in terms of measurement techniques and physical (transport) phenomena. The use of Pandora total and tropospheric NO2 VCDs for validation of collocated TROPOspheric Monitoring Instrument (TROPOMI) data, resampled to 100 m × 100 m, shows that although on average the TROPOMI VCDs are slightly lower, they are well within the expected error for TROPOMI of 0.5 Pmolec.cm-2 + (0.2 to 0.5) ⋅ VCDtrop (1 Pmolec.cm-2 = 1 × 1015 molec cm−2). The location of the Pandora instrument within a sub-orbital TROPOMI pixel of 3.5 km × 5.5 km may result in an error in the TROPOMI-derived tropospheric NO2 VCD between 0.223 and 0.282 Pmolec.cm-2, i.e., between 1.7 % and 2 %. In addition, the data also show that the Pandora observations at the Beijing-RADI site are representative of an area with a radius of 10 km.

Airborne observation with a low-cost hyperspectral instrument: retrieval of NO2 vertical column densities (VCDs) and the satellite sub-grid variability over industrial point sources

Abstract. High-spatial-resolution NO2 vertical column densities (VCDs) were retrieved from airborne observations using the low-cost hyperspectral imaging sensor (HIS) at three industrial areas (i.e., Chungnam, Jecheon, and Pohang) in South Korea, where point sources (i.e., power plant, petrochemical complex, steel yard, and cement kiln) with significant NO2 emissions are located. An innovative and versatile approach for NO2 VCD retrieval, hereafter referred to as the modified wavelength pair (MWP) method, was developed to overcome the excessively variable radiometric and spectral characteristics of the HIS attributed to the absence of temperature control during the flight. The newly developed MWP method was designed to be insensitive to broadband spectral features, including the spectral dependency of surface and aerosol reflectivity, and can be applied to observations with relatively low spectral resolutions. Moreover, the MWP method can be implemented without requiring precise radiometric calibration of the instrument (i.e., HIS) by utilizing clean-pixel data for non-uniformity corrections and is also less sensitive to the optical properties of the instrument and offers computational cost competitiveness. In the experimental flights using the HIS, NO2 plumes emitted from steel yards were particularly conspicuous among the various NO2 point sources, with peak NO2 VCDs of 2.0 DU (Dobson unit) at Chungnam and 1.8 DU at Pohang. Typical NO2 VCD uncertainties ranged between 0.025–0.075 DU over the land surface and 0.10–0.15 DU over the ocean surface, and the discrepancy can be attributable to the lower signal-to-noise ratio over the ocean and higher sensitivity of the MWP method to surface reflectance uncertainties under low-albedo conditions. The NO2 VCDs retrieved from the HIS with the MWP method showed a good correlation with the collocated Tropospheric Monitoring Instrument (TROPOMI) data (r=0.73, mean absolute error equals 0.106 DU). However, the temporal disparities between the HIS frames and the TROPOMI overpass, their spatial mismatch, and their different observation geometries could limit the correlation. The comparison of TROPOMI and HIS NO2 VCDs further demonstrated that the satellite sub-grid variability could be intensified near the point sources, with more than a 3-fold increase in HIS NO2 VCD variability (e.g., difference between 25th and 75th quantiles) over the TROPOMI footprints with NO2 VCD values exceeding 0.8 DU compared to footprints with NO2 VCD values below 0.6 DU.

On the influence of vertical mixing, boundary layer schemes, and temporal emission profiles on tropospheric NO2 in WRF-Chem – comparisons to in situ, satellite, and MAX-DOAS observations

Abstract. We present WRF-Chem simulations over central Europe with a spatial resolution of 3 km × 3 km and focus on nitrogen dioxide (NO2). A regional emission inventory issued by the German Environmental Agency, with a spatial resolution of 1 km × 1 km, is used as input. We demonstrate by comparison of five different model setups that significant improvements in model accuracy can be achieved by choosing the appropriate boundary layer scheme, increasing vertical mixing strength, and/or tuning the temporal modulation of the emission data (“temporal profiles”) driving the model. The model setup with improved vertical mixing is shown to produce the best results. Simulated NO2 surface concentrations are compared to measurements from a total of 275 in situ measurement stations in Germany, where the model was able to reproduce average noontime NO2 concentrations with a bias of ca. −3 % and R=0.74. The best agreement is achieved when correcting for the presumed NOy cross sensitivity of the molybdenum-based in situ measurements by computing an NOy correction factor from modelled peroxyacetyl nitrate (PAN) and nitric acid (HNO3) mixing ratios. A comparison between modelled NO2 vertical column densities (VCDs) and satellite observations from TROPOMI (TROPOspheric Monitoring Instrument) is conducted with averaging kernels taken into account. Simulations and satellite observations are shown to agree with a bias of +5.5 % and R=0.87 for monthly means. Lastly, simulated NO2 concentration profiles are compared to noontime NO2 profiles obtained from multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements at five locations in Europe. For stations within Germany, average biases of −25.3 % to +12.0 % were obtained. Outside of Germany, where lower-resolution emission data were used, biases of up to +50.7 % were observed. Overall, the study demonstrates the high sensitivity of modelled NO2 to the mixing processes in the boundary layer and the diurnal distribution of emissions.

TROPOMI NO2 Sentinel-5P data in the Community of Madrid: A detailed consistency analysis with in situ surface observations

Excess reactive nitrogen emissions from anthropogenic activities can negatively impact the natural environment. The sensor TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor (Sentinel-5P) satellite is capable of providing data on tropospheric NO2 vertical column densities (VCDs). This work investigates NO2 data retrieved from TROPOMI to study the spatial and temporal patterns of NO2 pollution compared with surface-level concentration measurements in the Community of Madrid in 2022. A high linear correlation coefficient (r) was obtained by comparing daily Level-3 tropospheric TROPOMI NO2 data with ground-based data from air quality monitoring stations at satellite overpass time (r = 0.78). Since the overpasses of Sentinel-5P over the region consistently occur between 12:00 and 4:00 p.m. local time, a second correlation analysis was carried out by averaging all available data from both sources within that interval, resulting in an even higher coefficient (r = 0.81). Results showed a lower correlation at rural sites compared to urban and suburban sites. Examining the monthly and weekly variations of NO2 concentration from satellite data and in situ measurements, similar tendencies in NO2 concentration were observed from both sources. In agreement with previous studies, the cold months and weekdays exhibited higher NO2 concentrations. It was concluded that TROPOMI NO2 data and in situ measurements yield a strong correlation for the Community of Madrid target area, and TROPOMI data can be further investigated to propose pollution mitigation policies.

Ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations of NO2 and H2CO at Kinshasa and comparisons with TROPOMI observations

Abstract. We present a database of MAX-DOAS (Multi-AXis Differential Optical Absorption Spectroscopy) ground-based observations of NO2 and H2CO tropospheric vertical column densities (VCDtropo) performed for the first time in the city of Kinshasa. These measurements were conducted between November 2019 and July 2021 and processed using the standardized inversion tools developed in the ESA FRM4DOAS (Fiducial Reference Measurements for Ground-Based DOAS Air-Quality Observations) project. The retrieved geophysical quantities are used to validate column observations from the TROPOspheric Monitoring Instrument (TROPOMI) over Kinshasa. In the validation, we experiment with three different comparison cases of increasing complexity. In the first case, a direct comparison between MAX-DOAS observations (hourly average of MAX-DOAS VCDtropo at overpass) and TROPOMI shows an underestimation of TROPOMI with a median bias of −38 % for NO2 and −39 % for H2CO based on monthly comparison. The second case takes into account the different vertical sensitivities of the two instruments and the a priori profile. We note significant changes in the median bias for both compounds: −12 % for NO2 and +11 % for H2CO. The third case builds on the second case by considering also the direction of sight of the MAX-DOAS. For this third case, we find a median bias of +44 % for NO2 and a median bias of +4 % for H2CO. However this case is impacted by low sampling and is considered less reliable. The findings from this study underscore the significance of employing a realistic a priori profile in TROPOMI column extraction, particularly within heavily polluted urban zones like Kinshasa. The investigation also highlights the necessity for prudence when integrating the MAX-DOAS line of sight due to the noise generated during subsampling and the limited horizontal sensitivity of MAX-DOAS observations. Importantly, the study further reveals the pronounced pollution levels of NO2, H2CO and aerosols in both the city of Kinshasa and its adjacent regions, underscoring the imperative for consistent monitoring and effective regulatory measures by local authorities.

Estimate of near-surface NO2 concentrations in Fenwei Plain, China, based on TROPOMI data and random forest model.

Nitrogen dioxide (NO2) concentration is a crucial indicator of ground-level air quality, and elevated concentrations can adversely affect human health and the atmospheric environment. In this study, we utilized Tropospheric Monitoring Instrument (TROPOMI) tropospheric NO2 vertical column density data (VCD) and multi-source geographic data to establish a random forest regression (RF) model that accurately estimates NO2 concentrations near the ground in the Fenwei Plain. The model addresses the inherent limitations of traditional ground-based monitoring and provides data support for analyzing regional pollution spatial and temporal characteristics. (1) The RF model based on TROPOMI and geographic data demonstrates high estimation accuracy, with monthly average RF model fit and validation coefficient of determination (R2) reaching 0.949 and 0.875, respectively. (2) A complex nonlinear relationship exists between near-surface NO2 concentration and multi-source geographic data. The RF model's estimations reveal clear seasonal and regional variations in near-surface NO2 concentration. Concentrations are generally highest in winter, followed by spring and autumn, and lowest in summer. The high NO2 concentrations are primarily mainly distributed in the plains and river valleys with low elevation and dense population density. The model estimation results also indicate that the estimated effect is better when the NO2 concentration fluctuates less and anthropogenic emission reduction measures significantly impact the NO2 concentration near the ground. (3) The population exposure risk results indicate that most cities in the Fenwei Plain face varying exposure risks. These findings offer valuable insights for regional NO2 pollution management.

Retrieval of Tropospheric NO2 Vertical Column Densities from Ground-Based MAX-DOAS Measurements in Lhasa, a City on the Tibetan Plateau

In order to investigate the abundance of and temporal variation in nitrogen dioxide (NO2) in the troposphere and validate the corresponding satellite products during a normal year and the lockdown period of coronavirus disease 2019 (COVID-19) in Lhasa, a city on the Tibetan Plateau (TP), ground-based remote-sensing measurements captured by applying multi-axis differential optical absorption spectroscopy (MAX-DOAS) were recorded from August 2021 to March 2023 at the Lhasa site (91.14°E, 29.66°N; 3552.5 m altitude). The NO2 differential slant column densities (dSCDs) were retrieved from the spectra of scattered solar light at different elevation angles. Then, the tropospheric NO2 vertical column densities (VCDs) were calculated with the geometric approximation method. Based on the retrieved tropospheric NO2 VCDs, we found that the pattern of monthly variation in tropospheric NO2 VCDs in Lhasa presented two peaks, one in winter and one around May. According to the monthly means of tropospheric NO2 VCDs during the COVID-19 lockdown, the NO2 background level in Lhasa was estimated to be 0.53 × 1015 molecules·cm−2. For diurnal variations in tropospheric NO2 VCDs, the morning and evening peaks disappeared during the COVID-19 lockdown period. The east–west direction (i.e., along the river valley) was the main path of NO2 transport and dispersion in Lhasa, but the tropospheric NO2 VCDs were little dependent on the wind direction or wind speed during the COVID-19 lockdown. The correlation coefficient of tropospheric NO2 VCDs was R = 0.33 (R = 0.43), with the averaged relative deviation of −28% (99%) for the TROPOMI (GEMS) relative to ground-based MAX-DOAS. The monthly deviations of tropospheric NO2 VCDs between ground-based MAX-DOAS and the satellite showed a dependence on NO2 abundance, with the maxima of the monthly positive deviations during the COVID-19 lockdown period. The GEMS could not capture the strong and systematic diurnal variation in tropospheric NO2 VCDs in the “normal” year well. During the COVID-19 lockdown, the GEMS (&gt;2 × 1015 molecules·cm−2) overestimated the hourly levels measured by ground-based MAX-DOAS (&lt;1.6 × 1015 molecules·cm−2). As a whole, these results are beneficial to understanding the influences of anthropogenic activities on NO2 background levels in Lhasa and to learning the accuracy of satellite products over the TP, with its high altitude and complex terrain.

A CNN-SVR model for NO2 profile prediction based on MAX-DOAS observations: The influence of Chinese New Year overlapping the 2020 COVID-19 lockdown on vertical distributions of tropospheric NO2 in Nanjing, China

In this study, a hybrid model, the convolutional neural network-support vector regression model, was adopted to achieve prediction of the NO2 profile in Nanjing from January 2019 to March 2021. Given the sudden decline in NO2 in February 2020, the contribution of the Coronavirus Disease-19 (COVID-19) lockdown, Chinese New Year (CNY), and meteorological conditions to the reduction of NO2 was evaluated. NO2 vertical column densities (VCDs) from January to March 2020 decreased by 59.05% and 32.81%, relative to the same period in 2019 and 2021, respectively. During the period of 2020 COVID-19, the average NO2 VCDs were 50.50% and 29.96% lower than those during the pre-lockdown and post-lockdown periods, respectively. The NO2 volume mixing ratios (VMRs) during the 2020 COVID-19 lockdown significantly decreased below 400 m. The NO2 VMRs under the different wind fields were significantly lower during the lockdown period than during the pre-lockdown period. This phenomenon could be attributed to the 2020 COVID-19 lockdown. The NO2 VMRs before and after the CNY were significantly lower in 2020 than in 2019 and 2021 in the same period, which further proves that the decrease in NO2 in February 2020 was attributed to the COVID-19 lockdown. Pollution source analysis of an NO2 pollution episode during the lockdown period showed that the polluted air mass in the Beijing-Tianjin-Hebei was transported southwards under the action of the north wind, and the subsequent unfavorable meteorological conditions (local wind speed of < 2.0 m/sec) resulted in the accumulation of pollutants.

First-time comparison between NO2 vertical columns from Geostationary Environmental Monitoring Spectrometer (GEMS) and Pandora measurements

Abstract. The Geostationary Environmental Monitoring Spectrometer (GEMS) is a UV-visible (UV-Vis) spectrometer on board the GEO-KOMPSAT-2B (Geostationary Korea Multi-Purpose Satellite 2B) satellite launched into a geostationary orbit in February 2020. To evaluate the GEMS NO2 total column data, a comparison was carried out using the NO2 vertical column density (VCD) that measured direct sunlight using the Pandora spectrometer system at four sites in Seosan, South Korea, from November 2020 to January 2021. Correlation coefficients between GEMS and Pandora NO2 data at four sites ranged from 0.35 to 0.48, with root mean square errors (RMSEs) from 4.7×1015 to 5.5×1015 molec. cm−2 for a cloud fraction (CF) &lt;0.7. Higher correlation coefficients of 0.62–0.78 with lower RMSEs from 3.3×1015 to 5.0×1015 molec. cm−2 were found with CF &lt;0.3, indicating the higher sensitivity of GEMS to atmospheric NO2 in less cloudy conditions. Overall, the GEMS NO2 total column data tended to be lower than the Pandora data, owing to differences in the representative spatial coverage, with a large negative bias under high CF conditions. With a correction for horizontal representativeness in the Pandora measurement coverage, correlation coefficients ranging from 0.69 to 0.81, with RMSEs from 3.2×1015 to 4.9×1015 molec. cm−2, were achieved for CF &lt;0.3, showing a better correlation with the correction than without the correction.

Long-term spatiotemporal variations in surface NO2 for Beijing reconstructed from surface data and satellite retrievals

Remote sensing data from the Ozone Monitoring Instrument (OMI) and the TROPOspheric Monitoring Instrument (TROPOMI) play important roles in estimating surface nitrogen dioxide (NO2), but few studies have compared their differences for application in surface NO2 reconstruction. This study aims to explore the effectiveness of incorporating the tropospheric NO2 vertical column density (VCD) from OMI and TROPOMI (hereafter referred to as OMI and TROPOMI, respectively, for conciseness) for deriving surface NO2 and to apply the resulting data to revisit the spatiotemporal variations in surface NO2 for Beijing over the 2005–2020 period during which there were significant reductions in nitrogen oxide emissions. In the OMI versus TROPOMI performance comparison, the cross-validation R2 values were 0.73 and 0.72, respectively, at 1 km resolution and 0.69 for both at 100 m resolution. The comparisons between satellite data sources indicate that even though TROPOMI has a finer resolution it does not improve upon OMI for deriving surface NO2 at 1 km resolution, especially for analyzing long-term trends. In light of the comparison results, we used a hybrid approach based on machine learning to derive the spatiotemporal distribution of surface NO2 during 2005–2020 based on OMI. We had novel, independent passive sampling data collected weekly from July to September of 2008 for hindcasting validation and found a spatiotemporal R2 of 0.46 (RMSE = 7.0 ppb). Regarding the long-term trend of surface NO2, the level in 2008 was obviously lower than that in 2007 and 2009, as expected, which was attributed to pollution restrictions during the Olympic Games. The NO2 level started to steadily decline from 2015 and fell below 2008's level after 2017. Based on OMI, a long-term and fine-resolution surface NO2 dataset was developed for Beijing to support future environmental management questions and epidemiological research.

Assessing the impact of urban form and urbanization process on tropospheric nitrogen dioxide pollution in the Yangtze River Delta, China

Optimizing urban form through urban planning and management policies can improve air quality and transition to demand-side control. Nitrogen dioxide (NO2) in the urban atmosphere, mainly emitted by anthropogenic sources such as industry and vehicles, is a key precursor of fine particles and ozone pollution. Both NO2 and its secondary pollutants pose health risks for humans. Here we assess the interactions between urban forms and airborne NO2 pollution in different cities with various stages of urbanization in the Yangtze River Delta (YRD) in China, by using the machine learning and geographical regression model. The results reveal a strong correlation between urban fragmentation and tropospheric NO2 vertical column density (TVCD) in YRD cities in 2020, particularly those with lower or higher levels of urbanization. The correlation coefficients (R2) between NO2 TVCD and the largest patch index (a metric of urban fragmentation) in different cities are greater than 0.8. For cities at other urbanization stages, population and road density are strongly correlated with NO2 TVCD, with an R2 larger than 0.61. This study highlights the interdependence among urbanization, urban forms, and air pollution, emphasizing the importance of customized urban landscape management strategies for mitigating urban air pollution.

Estimating surface-level nitrogen dioxide concentrations from Sentinel-5P/TROPOMI observations in Finland

In recent decades, satellite instruments have been providing observations of air pollutants such as nitrogen dioxide (NO2) with global coverage. Since late 2018, the TROPOspheric Monitoring Instrument (TROPOMI) on-board the Copernicus Sentinel-5 Precursor satellite has produced NO2 vertical column densities (VCDs) with the best spatial resolution (currently 5.5 × 3.5km2 at nadir). In this paper, we test and adapt two previously published methods to estimate surface-level NO2 concentrations from TROPOMI VCD retrievals in the specific conditions of Finland. Satellite-based estimates show good correlation with co-located surface NO2 measurements from the Finnish AQ network, although not accounting for the level of NO2 mixing within the boundary layer leads to underestimation. We also use a linear relation between in situ measurements and surface-level estimates to correct for the observed negative bias in the estimates. Finally, we use chemical transport model simulations to estimate the ratio of the annual mean surface concentrations to the values sampled according to TROPOMI observation times, and use it to correct our surface-level NO2 estimates for compatibility with annual limit values defined in AQ legislation.Overall, the results provide new information to complement traditional ground-based AQ measurements, especially over areas where the surface AQ networks are sparse, and to support national environmental authorities in air quality assessment and reporting.