Variable effects of spatial resolution on modeling of nitrogen oxides

Abstract

The lifetime and concentration of nitrogen oxides (NOx) are susceptible to nonlinear production and loss and to the resolution of a chemical transport model (CTM). This is due to the strong spatial gradients of NOx and the dependence of its own chemical loss on such gradients. In this study, we use the GEOS-Chem CTM in its high-performance implementation (GCHP) to investigate NOx simulations over the eastern United States across a wide range of spatial model resolutions (six different horizontal grids from 13 to 181gkm). Following increasing grid size, afternoon surface NOx mixing ratios over July 2015 generally decrease over the Great Lakes region (GL) and increase over the southern states of the US region (SS), yielding regional differences (181gkm vs. 13gkm) of-16g% (in the GL) to 7g% (in the SS); meanwhile, hydrogen oxide radicals (HOx) increase over both regions, consistent with their different chemical regimes (i.e., NOx-saturated in the GL and NOx-limited in the SS). Nighttime titration of ozone by surface nitric oxide (NO) was found to be more efficient at coarser resolutions, leading to longer NOx lifetimes and higher surface mixing ratios of nitrogen dioxide (NO2) over the GL in January 2015. The tropospheric NO2 column density at typical afternoon satellite overpass time has spatially more coherent negative biases (e.g.,-8g% over the GL) at coarser resolutions in July, which reversed the positive biases of surface NOx over the SS. The reduced NOx aloft (>1gkm altitude) at coarser resolutions was attributable to the enhanced HOx that intrudes into the upper troposphere. Application of coarse-resolution simulations for interpreting satellite NO2 columns will generally underestimate surface NO2 over the GL and overestimate surface NO2 over the SS in summer, but it will uniformly overestimate NOx emissions over both regions. This study significantly broadens understanding of factors contributing to NOx resolution effects and the role of fine-resolution data in accurately simulating and interpreting NOx and its relevance to air quality.