Seeded Crystal Growth of Internally Mixed Organic-Inorganic Aerosols: Impact of Organic Phase State.

Abstract

Atmospheric aerosols are complex with both inorganic and organic components. The soluble inorganics can transition between aqueous and crystalline phases through efflorescence and deliquescence. This study focuses on the efflorescence of (NH4)2SO4/organic particles by seeded crystal growth through contact with a crystal of (NH4)2SO4. Seeded crystal growth is known to effectively shut down supersaturation of aqueous aerosols. Here, we investigate whether organics can inhibit seeded crystal growth. We demonstrate that poly(ethylene glycol) 400 (PEG-400), which phase-separates from the aqueous (NH4)2SO4 and forms a core-shell structure, did not inhibit seeded crystal growth of (NH4)2SO4 at all relative humidity (RH) values below deliquescence RH. The PEG-400 layer was not viscous enough to prevent the diffusion of species through the coating. In contrast, we find that although raffinose, which stays homogeneously mixed with (NH4)2SO4, did not inhibit seeded crystal growth at RH > 45%, it did inhibit heterogeneous efflorescence at lower humidities. Viscosity measurements using an electrodynamic balance show a significant increase in viscosity as humidity was lowered, suggesting that inhibited diffusion of water and ions prevented efflorescence. The observed efflorescence at the higher RH also demonstrates that collisions can induce efflorescence of mixed aerosols that would otherwise not homogeneously effloresce.