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.
Original language | English (US) |
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Article number | 579 |
Pages (from-to) | 11263-11273 |
Number of pages | 11 |
Journal | Atmospheric Chemistry and Physics |
Volume | 20 |
Issue number | 19 |
DOIs | |
State | Published - Oct 2 2020 |
Funding
Financial support. This research has been supported by the Acknowledgements. For the authors at Jeonbuk National University, this work was supported by a National Research Foundation of Korea grant funded by the Korean Government (2019R1A2C1086187) and by a Research Base Construction Fund Support Program funded by Jeonbuk National University in 2020. Mijung Song gives thanks to Gwanggon Jo for the technical support. The US National Science Foundation (AGS-1640378) is acknowledged by the authors from Harvard University. The authors at Northwestern University acknowledge support from the US National Science Foundation (CHE-1607640 and Graduate Research Fellowship to AGB).
ASJC Scopus subject areas
- Atmospheric Science