Liquid-liquid phase separation in particles containing secondary organic material free of inorganic salts

Particles containing secondary organic material (SOM) are ubiquitous in the atmosphere and play a role in climate and air quality. Recently, research has shown that liquid-liquid phase separation (LLPS) occurs at high relative humidity (RH) (greater than similar to 95 %) in alpha-pinene-derived SOM particles free of inorganic salts, while LLPS does not occur in isoprene-derived SOM particles free of inorganic salts. We expand on these findings by investigating LLPS at 290 +/- 1K in SOM particles free of inorganic salts produced from ozonolysis of beta-caryophyllene, ozonolysis of limonene, and photo-oxidation of toluene. LLPS was observed at greater than similar to 95% RH in the biogenic SOM particles derived from beta-caryophyllene and limonene while LLPS was not observed in the anthropogenic SOM particles derived from toluene. This work combined with the earlier work on LLPS in SOM particles free of inorganic salts suggests that the occurrence of LLPS in SOM particles free of inorganic salts is related to the oxygen-to-carbon elemental ratio (O : C) of the organic material. These results help explain the difference between the hygroscopic parameter K of SOM particles measured above and below water saturation in the laboratory and field, and have implications for predicting the cloud condensation nucleation properties of SOM particles.