Global high-resolution simulations of tropospheric nitrogen dioxide using CHASER V4.0

Abstract

We evaluate global tropospheric nitrogen dioxide (NO2) simulations using the CHASER V4.0 global chemical transport model (CTM) at horizontal resolutions of 0.56, 1.1, and 2.8°. Model evaluation was conducted using satellite tropospheric NO2 retrievals from the Ozone Monitoring Instrument (OMI) and the Global Ozone Monitoring Experiment-2 (GOME-2) and aircraft observations from the 2014 Front Range Air Pollution and Photochemistry Experiment (FRAPPÉ). Agreement against satellite retrievals improved greatly at 1.1 and 0.56° resolutions (compared to 2.8° resolution) over polluted and biomass burning regions. The 1.1° simulation generally captured the regional distribution of the tropospheric NO2 column well, whereas 0.56° resolution was necessary to improve the model performance over areas with strong local sources, with mean bias reductions of 67g% over Beijing and 73g% over San Francisco in summer. Validation using aircraft observations indicated that high-resolution simulations reduced negative NO2 biases below 700ghPa over the Denver metropolitan area. These improvements in high-resolution simulations were attributable to (1) closer spatial representativeness between simulations and observations and (2) better representation of large-scale concentration fields (i.e., at 2.8°) through the consideration of small-scale processes. Model evaluations conducted at 0.5 and 2.8° bin grids indicated that the contributions of both these processes were comparable over most polluted regions, whereas the latter effect (2) made a larger contribution over eastern China and biomass burning areas. The evaluations presented in this paper demonstrate the potential of using a high-resolution global CTM for studying megacity-scale air pollutants across the entire globe, potentially also contributing to global satellite retrievals and chemical data assimilation.