Abstract

The hygroscopic properties of sulfate-containing particles are important to understanding the behavior of atmospheric aerosols. At high concentrations, chemical interactions between sulfate ions with the countercations are significant and lead to the formation of contact pairs. In this paper, Raman spectroscopy was used to study the structural changes of single aqueous droplets of equal molar Na2SO4/MgSO4 mixture, Na2SO4, (NH4)2SO4, MgSO4, ZnSO4, and CdSO4 in relation to their hygroscopic properties in an electrodynamic balance. The molar water-to-solute ratio (WSR) and the Raman spectra of droplets equilibrated at different ambient relative humidities were measured. When RH is reduced, the WSR of the Na2SO4/MgSO4 droplet decreases from 25.3 to 4.2 without crystallization but with two distinct transition points. The first one appears at WSR = 18.9, where the WSR is more sensitive to RH and the shoulder at 995 cm-1 of the ν1-SO42- band of the Raman spectrum shows an abrupt change in the ratio of the intens...

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