Assessment of the global impact of aerosols on tropospheric oxidants

Abstract

We present here a fully coupled global aerosol and chemistry model for the troposphere. The model is used to assess the interactions between aerosols and chemical oxidants in the troposphere, including (1) the conversion from gas‐phase oxidants into the condensed phase during the formation of aerosols, (2) the heterogeneous reactions occurring on the surface of aerosols, and (3) the effect of aerosols on ultraviolet radiation and photolysis rates. The present study uses the global three‐dimensional chemical/transport model, Model for Ozone and Related Chemical Tracers, version 2 (MOZART‐2), in which aerosols are coupled with the model. The model accounts for the presence of sulfate, soot, primary organic carbon, ammonium nitrate, secondary organic carbon, sea salt, and mineral dust particles. The simulated global distributions of the aerosols are analyzed and evaluated using satellite measurements (Moderate‐Resolution Imaging Spectroradiometer (MODIS)) and surface measurements. The results suggest that in northern continental regions the tropospheric aerosol loading is highest in Europe, North America, and east Asia. Sulfate, organic carbon, black carbon, and ammonium nitrate are major contributions for the high aerosol loading in these regions. Aerosol loading is also high in the Amazon and in Africa. In these areas the aerosols consist primarily of organic carbon and black carbon. Over the southern high‐latitude ocean (around 60°S), high concentrations of sea‐salt aerosol are predicted. The concentration of mineral dust is highest over the Sahara and, as a result of transport, spread out into adjacent regions. The model and MODIS show similar geographical distributions of aerosol particles. However, the model overestimates the sulfate and carbonaceous aerosol in the eastern United States, Europe, and east Asia. In the region where aerosol loading is high, aerosols have important impacts on tropospheric ozone and other oxidants. The model suggests that heterogeneous reactions of HO 2 and CH 2 O on sulfate have an important impact on HO x (OH + HO 2) concentrations, while the heterogeneous reaction of O 3 on soot has a minor effect on O 3 concentrations in the lower troposphere. The heterogeneous reactions on dust have very important impacts on HO x and O 3 in the region of dust mobilization, where the reduction of HO x and O 3 concentrations can reach a maximum of 30% and 20%, respectively, over the Sahara desert. Dust, organic carbon, black carbon, and sulfate aerosols have important impacts on photolysis rates. For example, the photodissociation frequencies of ozone and nitrogen dioxide are reduced by 20% at the surface in the Sahara, in the Amazon, and in eastern Asia, leading to 5–20% reduction in the concentration of HO x and to a few percent change in the O 3 abundance in these regions.