Spatial Distribution of Chemical Components in Aerosol Particles as Determined from Secondary Electron Yield Measurements: Implications for Mechanisms of Multicomponent Aerosol Crystallization

Abstract

Secondary electron yield measurements were used to determine the distribution of chemical components in multicomponent aerosol particles formed by crystallization from aqueous solution droplets. Yield measurements were made by measuring the charge acquired by a beam of particles as they passed through an electron beam (100–600 eV energy) inside a high-vacuum apparatus. Yields were sufficiently different for certain compounds that measurements made on two-component particles could be used to obtain information on the spatial distribution of components. Variations in chemical composition as a function of depth beneath the particle surface were ascertained from the energy dependence of the measured yields, since the electron penetration depth, and therefore the probe depth, increases with electron energy. The results for mixed NaCl–NH4Cl particles indicate that the distribution of components within these particles is relatively homogeneous, while measurements made on mixed NaCl–NaNO3particles are indicative of particles having a heterogeneous core–shell morphology. Results for mixed Na2SO4–(NH4)2SO4particles are ambiguous, probably because of the complexity of the phase diagram of this system. It appears that the mechanism by which aerosol particles crystallize, and therefore the resulting distribution of chemical components within particles, is strongly dependent on particle composition and environmental variables.