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Diesel-powered vehicles emit several times more nitrogen oxides than comparable gasoline-powered vehicles, leading to ambient nitrogen dioxide (NO2) pollution and adverse health impacts. The COVID-19 pandemic and ensuing changes in emissions provide a natural experiment to test whether NO2 reductions have been starker in regions of Europe with larger diesel passenger vehicle shares. Here we use a semi-empirical approach that combines in-situ NO2 observations from urban areas and an atmospheric composition model within a machine learning algorithm to estimate business-as-usual NO2 during the first wave of the COVID-19 pandemic in 2020. These estimates account for the moderating influences of meteorology, chemistry, and traffic. Comparing the observed NO2 concentrations against business-as-usual estimates indicates that diesel passenger vehicle shares played a major role in the magnitude of NO2 reductions. European cities with the five largest shares of diesel passenger vehicles experienced NO2 reductions ∼ 2.5 times larger than cities with the five smallest diesel shares. Extending our methods to a cohort of non-European cities reveals that NO2 reductions in these cities were generally smaller than reductions in European cities, which was expected given their small diesel shares. We identify potential factors such as the deterioration of engine controls associated with older diesel vehicles to explain spread in the relationship between cities’ shares of diesel vehicles and changes in NO2 during the pandemic. Our results provide a glimpse of potential NO2 reductions that could accompany future deliberate efforts to phase out or remove passenger vehicles from cities.

KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean Peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (24 May). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but overpredicted surface particulate matter concentrations in South Korea, especially PM2.5, often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low-resolution size bin representation (four bins) underestimates the efficiency with which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins (8–16 bins), it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve better consistency with measured values of the mass extinction efficiency (6.7 m2 g−1 observed average) and light-scattering enhancement factor (f(RH)) due to aerosol hygroscopic growth (2.2 observed average). Furthermore, an evaluation of the optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an underestimate of organic aerosol density (1.0 g cm−3 in the model vs. observed average of 1.5 g cm−3) and an overprediction of the fractional contribution of submicron inorganic aerosols other than sulfate, ammonium, nitrate, chloride, and sodium corresponding to mostly dust (17 %–28 % modeled vs. 12 % estimated from observations). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health impact assessments, climate projections, solar power forecasts, and aerosol data assimilation.

Fossil-fuel CO2 emissions and their trends in eight U.S. megacities during 2006–2017 are inferred by combining satellite-derived NOX emissions with bottom-up city-specific NOX-to-CO2 emission ratios. A statistical model is fit to a collection NO2 plumes observed from the Ozone Monitoring Instrument (OMI), and is used to calculate top-down NOX emissions. Decreases in OMI-derived NOX emissions are observed across the eight cities from 2006 to 2017 (−17% in Miami to −58% in Los Angeles), and are generally consistent with long-term trends of bottom-up inventories (−25% in Miami to −49% in Los Angeles), but there are some interannual discrepancies. City-specific NOX-to-CO2 emission ratios, used to calculate inferred CO2, are estimated through annual bottom-up inventories of NOX and CO2 emissions disaggregated to 1 × 1 km2 resolution. Over the study period, NOX-to-CO2 emission ratios have decreased by ~40% nationwide (−24% to −51% for our studied cities), which is attributed to a faster reduction in NOX when compared to CO2 due to policy regulations and fuel type shifts. Combining top-down NOX emissions and bottom-up NOX-to-CO2 emission ratios, annual fossil-fuel CO2 emissions are derived. Inferred OMI-based top-down CO2 emissions trends vary between +7% in Dallas to −31% in Phoenix. For 2017, we report annual fossil-fuel CO2 emissions to be: Los Angeles 113 ± 49 Tg/yr; New York City 144 ± 62 Tg/yr; and Chicago 55 ± 24 Tg/yr. A study in the Los Angeles area, using independent methods, reported a 2013–2016 average CO2 emissions rate of 104 Tg/yr and 120 Tg/yr, which suggests that the CO2 emissions from our method are in good agreement with other studies' top-down estimates. We anticipate future remote sensing instruments – with better spatial and temporal resolution – will better constrain the NOX-to-CO2 ratio and reduce the uncertainty in our method.