Nitrogen deposition to the United States: distribution, sources, and processes

Abstract

We simulate nitrogen deposition over the US in 2006–2008 by using the GEOS-Chem global chemical transport model at 1/2°×2/3° horizontal resolution over North America and adjacent oceans. US emissions of NO_x and NH₃ in the model are 6.7 and 2.9 Tg N a⁻¹ respectively, including a 20% natural contribution for each. Ammonia emissions are a factor of 3 lower in winter than summer, providing a good match to US network observations of NH_x (≡NH₃ gas + ammonium aerosol) and ammonium wet deposition fluxes. Model comparisons to observed deposition fluxes and surface air concentrations of oxidized nitrogen species (NO_y) show overall good agreement but excessive wintertime HNO₃ production over the US Midwest and Northeast. This suggests a model overestimate N₂O₅ hydrolysis in aerosols, and a possible factor is inhibition by aerosol nitrate. Model results indicate a total nitrogen deposition flux of 6.5 Tg N a⁻¹ over the contiguous US, including 4.2 as NO_y and 2.3 as NH_x. Domestic anthropogenic, foreign anthropogenic, and natural sources contribute respectively 78%, 6%, and 16% of total nitrogen deposition over the contiguous US in the model. The domestic anthropogenic contribution generally exceeds 70% in the east and in populated areas of the west, and is typically 50–70% in remote areas of the west. Total nitrogen deposition in the model exceeds 10 kg N ha⁻¹ a⁻¹ over 35% of the contiguous US.