Liquid–liquid phase separation and morphologies in organic particles consisting of iα/i-pinene and iβ/i-caryophyllene ozonolysis products and mixtures with commercially available organic compounds

摘要

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 one-component and two-component organic particles consisting of α-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:C) was ≤0.44 but did not occur when O: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:C ≤0.67 but never occurred when the average O: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.