Wet deposition of atmospheric selenium and sensitivity to emission and precipitation patterns.

ABSTRACT

Wet deposition has been well recognized to be affected by species concentration and precipitation; nevertheless, the regimes in the controlling factor of concentration or precipitation have not yet been clarified. Using a trace element, selenium (Se), with dual effects on human health as a testbed, we first reproduce the spatial distribution of atmospheric Se concentrations and wet deposition fluxes through GEOS-Chem on a global scale, and examine the spatial patterns and relative importance of anthropogenic emissions vs. natural emissions over various regions around the world. We find that over most Northern Hemisphere continental regions, anthropogenic emissions are the dominant source for atmospheric Se concentration and deposition, while it is dominated by natural sources in the other areas. Nested grid simulations covering China and the continental United States are further conducted. The factors (i.e., Se concentration and precipitation) controlling the wet deposition flux of atmospheric Se are analyzed in detail, through the construction of wet deposition-concentration-precipitation (WETD-C-P) diagram for two regions (mainland China and the continental United States) based on the monthly results. The two regions show distinctive features, reflecting the different spatial patterns of Se emissions and precipitation. Both Se emissions and precipitation are higher in the eastern United States than that in the western United States. In contrast, the emissions and precipitation in northern and southern China show dipole features with stronger emissions over the northern side and higher precipitation on the southern side. We further investigate the impacts of future emission changes in China on atmospheric Se deposition and its sensitivity to emissions and precipitation, revealing a modulation of regime shifts, i.e., from the precipitation dominant regime to the concurrent governance of both precipitation and emissions. The proposed WETD-C-P relationship is useful in elucidating the regime and factors governing the spatial and temporal variations in wet deposition.