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Nitrogen oxides (NOx = NO + NO2) play a crucial role in the formation of ozone and secondary inorganic and organic aerosols, thus affecting human health, global radiation budget, and climate. The diurnal and spatial variations in NO2 are functions of emissions, advection, deposition, vertical mixing, and chemistry. Their observations, therefore, provide useful constraints in our understanding of these factors. We employ a Regional chEmical and trAnsport model (REAM) to analyze the observed temporal (diurnal cycles) and spatial distributions of NO2 concentrations and tropospheric vertical column densities (TVCDs) using aircraft in situ measurements and surface EPA Air Quality System (AQS) observations as well as the measurements of TVCDs by satellite instruments (OMI: the Ozone Monitoring Instrument; GOME-2A: Global Ozone Monitoring Experiment – 2A), ground-based Pandora, and the Airborne Compact Atmospheric Mapper (ACAM) instrument in July 2011 during the DISCOVER-AQ campaign over the Baltimore–Washington region. The model simulations at 36 and 4 km resolutions are in reasonably good agreement with the regional mean temporospatial NO2 observations in the daytime. However, we find significant overestimations (underestimations) of model-simulated NO2 (O3) surface concentrations during nighttime, which can be mitigated by enhancing nocturnal vertical mixing in the model. Another discrepancy is that Pandora-measured NO2 TVCDs show much less variation in the late afternoon than simulated in the model. The higher-resolution 4 km simulations tend to show larger biases compared to the observations due largely to the larger spatial variations in NOx emissions in the model when the model spatial resolution is increased from 36 to 4 km. OMI, GOME-2A, and the high-resolution aircraft ACAM observations show a more dispersed distribution of NO2 vertical column densities (VCDs) and lower VCDs in urban regions than corresponding 36 and 4 km model simulations, likely reflecting the spatial distribution bias of NOx emissions in the National Emissions Inventory (NEI) 2011. [ABSTRACT FROM AUTHOR]

Nitrogen oxides (NOx = NO + NO2) play a crucial role in the formation of ozone and secondary inorganic and organic aerosols, thus affecting human health, global radiation budget, and climate. The diurnal and spatial variations of NO2 are functions of emissions, advection, deposition, vertical mixing, and chemistry. Their observations, therefore, provide useful constraints in our understanding of these factors. We employ a Regional chEmical and trAnsport model (REAM) to analyze the observed temporal (diurnal cycles) and spatial distributions of NO2 concentrations and tropospheric vertical column densities (TVCDs) using aircraft in situ measurements, surface EPA Air Quality System (AQS) observations, as well as the measurements of TVCDs by satellite instruments (OMI: the Ozone Monitoring Instrument; and GOME-2A: Global Ozone Monitoring Experiment - 2A), ground-based Pandora, and the Airborne Compact Atmospheric Mapper (ACAM) instrument, in July 2011 during the DISCOVER-AQ campaign over the Baltimore-Washington region. The model simulations at 36- and 4-km resolutions are in reasonably good agreement with the temporospatial NO2 observations in the daytime. However, nighttime mixing in the model needs to be enhanced to reproduce the observed NO2 diurnal cycle in the model. Another discrepancy is that Pandora measured NO2 TVCDs show much less variation in the late afternoon than simulated in the model. Relative to the 36-km model simulations, the 4-km model results show larger biases compared to the observations due largely to the larger spatial variations of NO2 in the model when the spatial resolution is increased from 36 to 4 km, although the biases are often comparable to the ranges of the observations. The high-resolution aircraft ACAM observations show a more dispersed distribution of NO2 vertical column densities (VCDs) and lower VCDs in urban regions than 4-km model simulations, reflecting likely the spatial distribution bias of NOx emissions in the National Emissions Inventory (NEI) 2011 at high resolution. [ABSTRACT FROM AUTHOR]

Airborne and ground-based Pandora spectrometer NO 2 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 NO 2 Tropospheric Vertical Column (TrVC) product v1.2 in this region, which has high spatial and temporal heterogeneity in NO 2. 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 (r2= 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 250 m × 250 m over the entire TROPOMI pixels they overfly. Thus, airborne data are more correlated with TROPOMI measurements (r2=0.96) than Pandora measurements are with TROPOMI (r2=0.84). The largest outliers between TROPOMI and the reference measurements appear to stem from too spatially coarse a priori surface reflectivity (0.5 ∘) 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 4 %–11 %. Excluding these cloud-impacted points, TROPOMI has an overall low bias of 19 %–33 % 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 these profiles with those from a 12 km North American Model–Community Multiscale Air Quality (NAMCMAQ) analysis results in a 12 %–14 % increase in the TrVCs. Even with this improvement, the TROPOMI-NAMCMAQ TrVCs have a 7 %–19 % 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. [ABSTRACT FROM AUTHOR]

Abundant NO[sub 2] column measurements from airborne and ground-based Pandora spectrometers were collected as part of the 2018 Long Island Sound Tropospheric Ozone Study (LISTOS) in the New York City/Long Island Sound region and coincided with early measurements from the Sentinel-5P TROPOMI instrument. Both airborne- and ground-based measurements are used to evaluate the TROPOspheric Monitoring Instrument (TROPOMI) NO[sub 2] Tropospheric Vertical Column (TrVC) product v1.2 in this region, which has high spatial and temporal heterogeneity in NO[sub 2]. 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 (r[sup 2]=0.92 and slope of 1.03) with the biggest 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 representivity. Pandora spectrometers can provide continuous long-term measurements but may lack areal representivity 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 250 m × 250 m over the entire TROPOMI pixels they overfly. Thus, airborne data are more correlated with TROPOMI measurements (r[sup 2]=0.96) than Pandora measurements are with TROPOMI (r[sup 2]=0.84). The largest outliers between TROPOMI and the reference measurements are caused by errors in the TROPOMI retrieval of cloud pressure impacting the calculation of tropospheric air mass factors in cloud-free scenes. This factor causes a high bias in TROPOMI TrVCs of 4-11 %. Excluding these cloud-impacted points, TROPOMI has an overall low bias of 19-33% during the LISTOS timeframe of June-September 2018. Part of this low bias is caused by coarse a priori profile input from TM5-MP model; replacing these profiles with those from a 12 km NAMCMAQ analysis results in a 12-14 % increase in the TrVCs. Even with this improvement, the TROPOMI-NAMCMAQ TrVCs have a 7-19 % 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. [ABSTRACT FROM AUTHOR]

NASA deployed the GeoTASO airborne UV–visible spectrometer in May–June 2017 to produce high-resolution (approximately 250m×250m) gapless NO2 datasets over the western shore of Lake Michigan and over the Los Angeles Basin. The results collected show that the airborne tropospheric vertical column retrievals compare well with ground-based Pandora spectrometer column NO2 observations (r2=0.91 and slope of 1.03). Apparent disagreements between the two measurements can be sensitive to the coincidence criteria and are often associated with large local variability, including rapid temporal changes and spatial heterogeneity that may be observed differently by the sunward-viewing Pandora observations. The gapless mapping strategy executed during the 2017 GeoTASO flights provides data suitable for averaging to coarser areal resolutions to simulate satellite retrievals. As simulated satellite pixel area increases to values typical of TEMPO (Tropospheric Emissions: Monitoring Pollution), TROPOMI (TROPOspheric Monitoring Instrument), and OMI (Ozone Monitoring Instrument), the agreement with Pandora measurements degraded, particularly for the most polluted columns as localized large pollution enhancements observed by Pandora and GeoTASO are spatially averaged with nearby less-polluted locations within the larger area representative of the satellite spatial resolutions (aircraft-to-Pandora slope: TEMPO scale =0.88 ; TROPOMI scale =0.77 ; OMI scale =0.57). In these two regions, Pandora and TEMPO or TROPOMI have the potential to compare well at least up to pollution scales of 30×1015 molecules cm -2. Two publicly available OMI tropospheric NO2 retrievals are found to be biased low with respect to these Pandora observations. However, the agreement improves when higher-resolution a priori inputs are used for the tropospheric air mass factor calculation (NASA V3 standard product slope =0.18 and Berkeley High Resolution product slope =0.30). Overall, this work explores best practices for satellite validation strategies with Pandora direct-sun observations by showing the sensitivity to product spatial resolution and demonstrating how the high-spatial-resolution NO2 data retrieved from airborne spectrometers, such as GeoTASO, can be used with high-temporal-resolution ground-based column observations to evaluate the influence of spatial heterogeneity on validation results. [ABSTRACT FROM AUTHOR]

NASA deployed an airborne UV/Visible spectrometer, GeoTASO, in May-June 2017 to produce high resolution (approximately 250 x 250 m), gapless NO2 datasets over the western shore of Lake Michigan and over the Los Angeles Basin. Results show that the airborne tropospheric vertical column retrievals compare well with ground-based Pandora spectrometer column NO2 observations (r² = 0.91 and slope of 1.03). Apparent disagreements between the two measurements can be sensitive to the coincidence criteria and are often associated with large local variability, including rapid temporal changes and also spatial heterogeneity that may be observed differently by the sunward viewing Pandora observations. The gapless mapping strategy executed during the 2017 GeoTASO flights provides data suitable for averaging to coarser areal resolutions to simulate satellite retrievals. As simulated satellite pixel area increases to values typical of TEMPO, TROPOMI, and OMI, the agreement with Pandora measurements is degraded as localized polluted plumes observed by Pandora are spatially averaged over larger areas (aircraft-to-Pandora slope: TEMPO scale = 0.88; TROPOMI scale = 0.77; OMI scale = 0.57). This behavior suggests that satellite products are representative of individual Pandora observations up to a certain pollution scale that depends on satellite spatial resolution. In these two regions, Pandora and TEMPO or TROPOMI have the potential to compare well up to pollution scales of 30 x 1015 molecules cm-2. Two publicly available OMI tropospheric NO2 retrievals are both found to be biased low with respect to Pandora observations (NASA V3 Standard Product slope = 0.18 and Berkeley High Resolution Product slope = 0.30). However, the agreement improves when higher resolution a priori inputs are used for the tropospheric air mass factor calculation. Overall, this work explores best practices for satellite validation strategies by showing the sensitivity to product spatial resolution and demonstrates how the high spatial resolution NO2 data retrieved from airborne spectrometers, such as GeoTASO, can be used with high temporal resolution surface observations to evaluate the influence of spatial heterogeneity on validation results. [ABSTRACT FROM AUTHOR]

The GEOstationary Coastal and Air Pollution Events (GEO-CAPE) Airborne Simulator (GCAS) was developed in support of NASA's decadal survey GEO-CAPE geostationary satellite mission. GCAS is an airborne push-broom remote-sensing instrument, consisting of two channels which make hyperspectral measurements in the ultraviolet/visible (optimized for air quality observations) and the visible–near infrared (optimized for ocean color observations). The GCAS instrument participated in its first intensive field campaign during the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign in Texas in September 2013. During this campaign, the instrument flew on a King Air B-200 aircraft during 21 flights on 11 days to make air quality observations over Houston, Texas. We present GCAS trace gas retrievals of nitrogen dioxide (NO2) and formaldehyde (CH2O), and compare these results with trace gas columns derived from coincident in situ profile measurements of NO2 and CH2O made by instruments on a P-3B aircraft, and with NO2 observations from ground-based Pandora spectrometers operating in direct-sun and scattered light modes. GCAS tropospheric column measurements correlate well spatially and temporally with columns estimated from the P-3B measurements for both NO2 (r2=0.89) and CH2O (r2=0.54) and with Pandora direct-sun (r2=0.85) and scattered light (r2=0.94) observed NO2 columns. Coincident GCAS columns agree in magnitude with NO2 and CH2O P-3B-observed columns to within 10 % but are larger than scattered light Pandora tropospheric NO2 columns by 33 % and direct-sun Pandora NO2 columns by 50 %. [ABSTRACT FROM AUTHOR]

The Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument is a test bed for upcoming air quality satellite instruments that will measure backscattered ultraviolet, visible and near-infrared light from geostationary orbit. GeoTASO flew on the NASA Falcon aircraft in its first intensive field measurement campaign during the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) Earth Venture Mission over Houston, Texas, in September 2013. Measurements of backscattered solar radiation between 420 and 465 nm collected on 4 days during the campaign are used to determine slant column amounts of NO2 at 250m?250m spatial resolution with a fitting precision of 2.2?1015 moleculescm-2. These slant columns are converted to tropospheric NO2 vertical columns using a radiative transfer model and trace gas profiles from the Community Multiscale Air Quality (CMAQ) model. Total column NO2 from GeoTASO is well correlated with ground-based Pandora observations (r = 0:90 on the most polluted and cloud-free day of measurements and r = 0:74 overall), with GeoTASO NO2 slightly higher for the most polluted observations. Surface NO2 mixing ratios inferred from GeoTASO using the CMAQ model show good correlation with NO2 measured in situ at the surface during the campaign (r = 0:85). NO2 slant columns from GeoTASO also agree well with preliminary retrievals from the GEO-CAPE Airborne Simulator (GCAS) which flew on the NASA King Air B200 (r = 0:81, slope = 0.91). Enhanced NO2 is resolvable over areas of traffic NOx emissions and near individual petrochemical facilities. [ABSTRACT FROM AUTHOR]

Nitrogen oxides (NOx = NO + NO2), produced in urban areas and industrial facilities (particularly in fossil fuel-fired power plants), are major sources of air pollutants, with implications for human health, leading local and national authorities to estimate their emissions using inventories. In Qatar, these inventories are not systematically updated, while the country is experiencing fast economic growth. Here, we use spaceborne retrievals of nitrogen dioxide (NO2) columns at high spatial resolution from the TROPOMI instrument to estimate NOx emissions in Qatar from 2019 to 2022 with a flux-divergence scheme, according to which emissions are calculated as the sum of a transport term and a sink term representing the three-body reaction comprising NO2 and hydroxyl radical (OH). Our results highlight emissions from gas power plants in the north-east of the country, and from the urban area of the capital Doha. The emissions from cement plants in the west and different industrial facilities in the south-east are under-estimated, due to frequent low-quality measurements of NO2 columns in these areas. Our top-down model estimates a weekly cycle with lower emissions on Fridays compared to the rest of the week, which is consistent with social norms in the country, and an annual cycle with mean emissions of 9.56 kt per month for the four-year period. These monthly emissions differ from CAMS-GLOB-ANT_v5.3 and EDGARv6.1 global inventories, for which the annual cycle is less marked and the average emissions are respectively 1.44 and 1.68 times higher. Our emission estimates are correlated with local electricity generation, and allow to infer a mean NOx emission factor of 0.557 tNOx.GWh−1 for the three gas power plants in the Ras Laffan area. [ABSTRACT FROM AUTHOR]