Liquid-liquid phase separation in organic particles containing one and two organic species: Importance of the average O:C

Recently, experimental studies have shown that liquid-liquid phase separation (LLPS) can occur in organic particles free of inorganic salts. Most of these studies used organic particles consisting of secondary organic materials generated in environmental chambers. To gain additional insight into LLPS in organic particles free of inorganic salts, we studied LLPS in organic particles consisting of one and two commercially available organic species. For particles containing one organic species, three out of the six particle types investigated underwent LLPS. In these cases, LLPS was observed when the O:C was ≤ 0.44 (but not always) and the relative humidity (RH) was between 97% and 100%. The mechanism of phase separation was likely nucleation and growth. For particles containing two organic species, 13 out of the 15 particle types investigated underwent LLPS. In these cases, LLPS was observed when the O:C was ≤ 0.58 (but not always) and mostly when the RH was between 90% RH and 100% RH. The mechanism of phase separation was likely spinodal decomposition. In almost all cases when LLPS was observed (for both one-component and two-component particles), the highest RH at which two liquids was observed was 100±2.0%, which has important implications for the cloud condensation nuclei (CCN) properties of these particles. These combined results provide additional evidence that LLPS needs to be considered when predicting the CCN properties of organic particles in the atmosphere.