Effects of mineral dust on global atmospheric nitrate concentrations

Abstract

Abstract. This study provides an assessment of the chemical composition and global aerosol load of the major inorganic aerosol components and determines the effect of mineral dust on their formation, focusing on aerosol nitrate. To account for this effect, the mineral dust aerosol components (i.e., Ca2+, Mg2+, K+, Na+) and their emissions are added to the ECHAM5/MESSy Atmospheric Chemistry model (EMAC). Gas/aerosol partitioning is simulated using the ISORROPIA-II thermodynamic equilibrium model that considers the interactions of K+-Ca2+-Mg2+-NH4+-Na+-SO42−-NO3−-Cl−-H2O aerosol components. Emissions of mineral dust aerosol components (K+-Ca2+-Mg2+-Na+) are calculated online by taking into account the soil particle size distribution and chemical composition of different deserts worldwide. The presence of the metallic ions on the simulated suite of components can substantially affect the nitrate partitioning into the aerosol phase due to thermodynamic interactions. The updated model improved the nitrate predictions over remote areas and found that the fine aerosol nitrate concentration is highest over urban and industrialized areas (1–3 μg m−3), while coarse aerosol nitrate is highest close to deserts (1–4 μg m−3). The contribution of mineral dust components to nitrate formation is large in areas with high dust concentrations with impacts that can extend across southern Europe, western USA and northeastern China. The tropospheric burden of aerosol nitrate increases by 44% by considering the interactions of nitrate with mineral dust cations. The calculated global average nitrate aerosol concentration near the surface increases by 36% while the coarse and fine mode concentrations of nitrate increase by 53 and 21%, respectively. Sensitivity tests show that nitrate aerosol formation is most sensitive to the chemical composition of the emitted mineral dust, followed by the soil size distribution of dust particles, the magnitude of the mineral dust emissions, and the aerosol state assumption.