Long-term trends in total inorganic nitrogen and sulfur deposition in the US from 1990 to 2010

Abstract

Abstract. Excess deposition (including both wet and dry deposition) of nitrogen and sulfur is detrimental to ecosystems. Recent studies have investigated the spatial patterns and temporal trends of nitrogen and sulfur wet deposition, but few studies have focused on dry deposition due to the scarcity of dry deposition measurements. Here, we use long-term model simulations from the coupled Weather Research and Forecasting and the Community Multiscale Air Quality (WRF-CMAQ) model covering the period from 1990 to 2010 to study changes in spatial distribution as well as temporal trends in total (TDEP), wet (WDEP), and dry deposition (DDEP) of total inorganic nitrogen (TIN) and sulfur (TS) in the United States (US). We first evaluate the model's performance in simulating WDEP over the US by comparing the model results with observational data from the US National Atmospheric Deposition Program. The coupled model generally underestimates the WDEP of both TIN (including both the oxidized nitrogen deposition, TNO3, and the reduced nitrogen deposition, NHx) and TS, with better performance in the eastern US than the western US. The underestimation of the wet deposition by the model is mainly caused by the coarse model grid resolution, missing lightning NOx emissions, and the poor temporal and spatial representation of NH3 emissions. TDEP of both TIN and TS shows significant decreases over the US, especially in the east, due to the large emission reductions that occurred in that region. The decreasing trends of TIN TDEP are caused by decreases in TNO3, and the increasing trends of TIN deposition over the Great Plains and Tropical Wet Forests (Southern Florida Coastal Plain) regions are caused by increases in NH3 emissions, although it should be noted that these increasing trends are not significant. TIN WDEP shows decreasing trends throughout the US, except for the Marine West Coast Forest region. TIN DDEP shows significant decreasing trends in the Eastern Temperate Forests, Northern Forests, Mediterranean California, and Marine West Coast Forest and significant increasing trends in the Tropical Wet Forests, Great Plains and Southern Semi-arid Highlands. For the other three regions (North American Deserts, Temperate Sierras, and Northwestern Forested Mountains), the decreasing or increasing trends are not significant. Both the WDEP and DDEP of TS have decreases across the US, with a larger decreasing trend in the DDEP than that in the WDEP. Across the US during the 1990–2010 period, DDEP of TIN accounts for 58–65 % of TDEP of TIN. TDEP of TIN over the US is dominated by deposition of TNO3 during the first decade, which then shifts to reduced nitrogen (NHx) dominance after 2003, resulting from a combination of NOx emission reductions and NH3 emission increases. The sulfur DDEP is usually higher than the sulfur WDEP until recent years, as the sulfur DDEP has a larger decreasing trend than WDEP.