Liquid-liquid phase separation and morphologies in organic particles consisting of α-pinene and β-caryophyllene ozonolysis products and mixtures with commercially available organic compounds

Abstract

Liquid-liquid phase separation (LLPS) in organic aerosol particles can impact several properties of atmospheric particulate matter, such as cloud condensation nuclei (CCN) properties, optical properties, and gas-to-particle partitioning. Yet, our understanding of LLPS in organic aerosols is far from complete. Here, we report on the LLPS of onecomponent and two-component organic particles consisting of a-pinene-and β-caryophyllene-derived ozonolysis products and commercially available organic compounds of relevance to atmospheric organic particles. In the experiments involving single-component organic particles, LLPS was observed in 8 out of 11 particle types studied. LLPS almost always occurred when the oxygen-to-carbon elemental ratio (O V C) was < 0.44 but did not occur when O V C was > 0.44. The phase separation occurred by spinodal decomposition as well as the nucleation and growth mechanism, and when LLPS occurred, two liquid phases coexisted up to ∼ 100 % relative humidity (RH). In the experiments involving two-component organic particles, LLPS was observed in 23 out of 25 particles types studied. LLPS almost always occurred when the average was O V C = 0.67 but never occurred when the average O V C was > 0.67. The phase separation occurred by spinodal decomposition as well as the nucleation and growth mechanism. When LLPS occurred, two liquid phases coexisted up to ∼ 100 % RH. These results provide further evidence that LLPS is likely a frequent occurrence in organic aerosol particles in the troposphere, even in the absence of inorganic salts.