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The COVID-19 pandemic created an extreme natural experiment in which sudden changes in human behavior and economic activity resulted in significant declines in nitrogen oxide (NOx) emissions, immediately after strict lockdowns were imposed. Here we examined the impact of multiple waves and response phases of the pandemic on nitrogen dioxide (NO2) dynamics and the role of meteorology in shaping relative contributions from different emission sectors to NO2 pollution in post-pandemic New York City. Long term (> 3.5 years), high frequency measurements from a network of ground-based Pandora spectrometers were combined with TROPOMI satellite retrievals, meteorological data, mobility trends, and atmospheric transport model simulations to quantify changes in NO2 across the New York metropolitan area. The stringent lockdown measures after the first pandemic wave resulted in a decline in top-down NOx emissions by approx. 30 % on top of long-term trends, in agreement with sector-specific changes in NOx emissions. Ground-based measurements showed a sudden drop in total column NO2 in spring 2020, by up to 36 % in Manhattan and 19 %–29 % in Queens, New Jersey (NJ), and Connecticut (CT), and a clear weakening (by 16 %) of the typical weekly NO2 cycle. Extending our analysis to more than a year after the initial lockdown captured a gradual recovery in NO2 across the NY/NJ/CT tri-state area in summer and fall 2020, as social restrictions eased, followed by a second decline in NO2 coincident with the second wave of the pandemic and resurgence of lockdown measures in winter 2021. Meteorology was not found to have a strong NO2 biassing effect in New York City after the first pandemic wave. Winds, however, were favorable for low NO2 conditions in Manhattan during the second wave of the pandemic, resulting in larger column NO2 declines than expected based on changes in transportation emissions alone. Meteorology played a key role in shaping the relative contributions from different emission sectors to NO2 pollution in the city, with low-speed (< 5 m s−1) SW-SE winds enhancing contributions from the high-emitting power-generation sector in NJ and Queens and driving particularly high NO2 pollution episodes in Manhattan, even during – and despite – the stringent early lockdowns. These results have important implications for air quality management in New York City, and highlight the value of high resolution NO2 measurements in assessing the effects of rapid meteorological changes on air quality conditions and the effectiveness of sector-specific NOx emission control strategies.

Airborne and ground-based Pandora spectrometer NO2 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 NO2 Tropospheric Vertical Column (TrVC) product v1.2 in this region, which has high spatial and temporal heterogeneity in NO2. 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.

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./.

NASA deployed the GeoTASO airborne UV–visible spectrometer in May–June 2017 to produce high-resolution (approximately 250 m×250 m) 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.

Determining effective strategies for mitigating surface ozone (O3) pollution requires knowledge of the relative ambient concentrations of its precursors, NOx, and VOCs. The space-based tropospheric column ratio of formaldehyde to NO2 (FNR) has been used as an indicator to identify NOx-limited versus NOx-saturated O3 formation regimes. Quantitative use of this indicator ratio is subject to three major uncertainties: (1) the split between NOx-limited and NOx-saturated conditions may shift in space and time, (2) the ratio of the vertically integrated column may not represent the near-surface environment, and (3) satellite products contain errors. We use the GEOS-Chem global chemical transport model to evaluate the quantitative utility of FNR observed from the Ozone Monitoring Instrument over three northern midlatitude source regions. We find that FNR in the model surface layer is a robust predictor of the simulated near-surface O3 production regime. Extending this surface-based predictor to a column-based FNR requires accounting for differences in the HCHO and NO2 vertical profiles. We compare four combinations of two OMI HCHO and NO2 retrievals with modeled FNR. The spatial and temporal correlations between the modeled and satellite-derived FNR vary with the choice of NO2 product, while the mean offset depends on the choice of HCHO product. Space-based FNR indicates that the spring transition to NOx-limited regimes has shifted at least a month earlier over major cities (e.g., New York, London, and Seoul) between 2005 and 2015. This increase in NOx sensitivity implies that NOx emission controls will improve O3 air quality more now than it would have a decade ago.

The atmospheric chemistry of cities depends strongly on the concentration of the hydroxyl radical (OH). OH removes organic molecules (τ = minutes - days), nitrogen oxides (NOx: NO + NO2; τ = 2 - 20 h), and sulfur dioxide (τ = 2 - 3 d) from the atmosphere and forms ozone and particulate matter in the process. The spatial and temporal variability of OH is not fully understood due in large part to its strong nonlinear dependence on the concentration of NOx. In this dissertation, I use measurements of the NO2 column from the Ozone Monitoring Instrument (OMI), a satellite-based UV/Visible spectrometer, and calculations from chemical transport models to investigate the relationship of OH and NOx in urban regions. I characterize the instrumental and model performance necessary to accurately infer OH concentration from space-based measurements of the NO2 column. I use the OMI observations and the WRF Chem model to investigate the spatial variability of the NO2 column over a variety of emission sources. I find, not surprisingly, that a result of the nonlinear dependence of OH on NOx is that the lifetime of NOx depends on the spatial distribution of NOx. Where the nonlinear NOx-OH feedbacks are most important, I find that a spatial resolution of 4 - 8 km is necessary for both model simulations and measurements to accurately capture variations of the NO2 column. Although this result is expected, quantitative analyses of the nonlinear coupling were not previously available and the calculations presented in this dissertation serve as a guide to interpretation of coarse-resolution measurements and models. I investigate the response of the NO2 column observed by OMI to variations of wind speed and day-of-week emission patterns. I find that these high spatial resolution measurements (13 × 24 km2 at nadir) contain independent information on both NOx emissions and removal.