Abstract
The chemical history of dust particles in the atmosphere is crucial for assessing their impact on both the Earth's climate and ecosystem. So far, a number of studies have shown that, in the vicinity of strong anthropogenic emission sources, Ca-rich dust particles can be converted into aqueous droplets mainly by the reaction with gaseous HNO(3) to form Ca(NO(3))(2). Here we show that other similar processes have the potential to be activated under typical remote marine atmospheric conditions. Based on field measurements at several sites in East Asia and thermodynamic predictions, we examined the possibility for the formation of two highly soluble calcium salts, Ca(NO(3))(2) and CaCl(2), which can deliquesce at low relative humidity. According to the results, the conversion of insoluble CaCO(3) to Ca(NO(3))(2) tends to be dominated over urban and industrialized areas of the Asian continent, where the concentrations of HNO(3) exceed those of HCl ([HNO(3)/HCl] > ∼ 1). In this regime, CaCl(2) is hardly detected from dust particles. However, the generation of CaCl(2) becomes detectable around the Japan Islands, where the concentrations of HCl are much higher than those of HNO(3) ([HNO(3)/HCl] < ∼ 0.3). We suggest that elevated concentrations of HCl in the remote marine boundary layer are sufficient to modify Ca-rich particles in dust storms and can play a more important role in forming a deliquescent layer on the particle surfaces as they are transported toward remote ocean regions.