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Liquid-liquid phase separation in atmospherically relevant particles You, Yuan

Abstract

Aerosol particles containing both organic material and inorganic salts are abundant in the atmosphere. These particles may undergo phase transitions when the relative humidity fluctuates between high and low values in the atmosphere. This dissertation focuses on liquid-liquid phase separation in atmospherically relevant mixed organic-inorganic salt particles. Liquid-liquid phase separation has potentially important implications in chemical and physical processes in the atmosphere. A humidity and temperature controlled flow cell coupled to either an optical, fluorescence, or Raman microscope was used to study the occurrence of liquid-liquid phase separation and the phase separation relative humidity (SRH) of particles containing atmospherically relevant organic species mixed with inorganic salts. Organic species in the particles studied include single organic species, such as carboxylic acids, alcohols, and oxidized aromatic compounds, as well as complex laboratory-produced secondary organic material. Material directly collected from the atmospheric environment was also studied. In this dissertation, the effects of oxygen-to-carbon elemental ratio (O:C) of the organic species, salt types, molecular weight of the organic species, and temperature on the occurrence of liquid-liquid phase separation and SRH were studies. The oxygenic-to-carbon elemental ratio was a useful parameter for predicting liquid-liquid phase separation and SRH. Liquid-liquid phase separation did not depend strongly on the molecular weight of the organic species or temperature. The correlation between SRH and O:C in particles containing organic species mixed with different salts were qualitatively similar. Results of this research will help improve the understanding of liquid-liquid phase separation in the atmospheric aerosols, and may, in turn, improve simulations and predictions of atmospheric chemistry and climate. Supplementary materials: http://hdl.handle.net/2429/50970

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