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Preprints
https://doi.org/10.5194/acp-2020-318
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-318
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  09 Apr 2020

09 Apr 2020

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A revised version of this preprint is currently under review for the journal ACP.

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

Young-Chul Song1, Ariana G. Bé2, Scot T. Martin3, Franz M. Geiger2, Allan K. Bertram4, Regan J. Thomson2, and Mijung Song1 Young-Chul Song et al.
  • 1Department of Earth and Environmental Sciences, Jeonbuk National University, Jeollabuk-do, Republic of Korea
  • 2Department of Chemistry, NorthwesternUniversity, Evanston, Illinois 60208, USA
  • 3Schoolof Engineering and Applied Sciences & Department of Earth and Planetary Sciences, Harvard University, Cambridge, Massachusetts 02138, USA
  • 4Department of Chemistry, University of British Columbia, Vancouver, BC, V6T 1Z1, Canada

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 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, and when LLPS occurred, two liquid phases co-existed 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 or growth of a second phase at the surface of the particles. When LLPS occurred, two liquid phases co-existed up to ~ 100 %. 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.

Young-Chul Song et al.

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Young-Chul Song et al.

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Short summary
We report on LLPS of organic aerosol consisting of α-pinene- and β-caryophyllene-derived ozonolysis products and commercial organic compounds. Our results show that as compositional complexity increased from one to two organic species, LLPS occurred over a wider range of average O : C values of organic materials (increasing from 0.44 to 0.67). These results provide further evidence that LLPS is likely a frequent occurrence in OA particles in the troposphere, even in the absence of inorganic salt.
We report on LLPS of organic aerosol consisting of α-pinene- and β-caryophyllene-derived...
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