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Title: Liquid–liquid phase separation in particles containing secondary organic material free of inorganic salts

Journal Article · · Atmospheric Chemistry and Physics (Online)
 [1]; ORCiD logo [2];  [3]; ORCiD logo [4]
  1. Chonbuk National Univ., Jeollabuk-do (Korea, Republic of). Dept. of Earth and Environmental Sciences; Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Chemistry
  2. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences
  3. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences; Harvard Univ., Cambridge, MA (United States). Dept. of Earth and Planetary Sciences
  4. Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Chemistry

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 ~95 %) in α-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 ± 1 K in SOM particles free of inorganic salts produced from ozonolysis of β-caryophyllene, ozonolysis of limonene, and photo-oxidation of toluene. LLPS was observed at greater than ~95 % RH in the biogenic SOM particles derived from β-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 κ 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.

Research Organization:
Harvard Univ., Cambridge, MA (United States)
Sponsoring Organization:
USDOE; Natural Sciences and Engineering Research Council of Canada (NSERC); National Science Foundation (NSF); National Research Foundation of Korea (NRF)
Grant/Contract Number:
SC0012792
OSTI ID:
1425661
Journal Information:
Atmospheric Chemistry and Physics (Online), Vol. 17, Issue 18; ISSN 1680-7324
Publisher:
European Geosciences UnionCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 38 works
Citation information provided by
Web of Science

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Cited By (7)

Multiphase reactivity of polycyclic aromatic hydrocarbons is driven by phase separation and diffusion limitations journal May 2019
Liquid–liquid phase separation in organic particles containing one and two organic species: importance of the average O : C journal January 2018
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors journal January 2019
A review of experimental techniques for aerosol hygroscopicity studies journal January 2019
Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter journal October 2018
Liquid–liquid phase separation and morphologies in organic particles consisting of <i>α</i>-pinene and <i>β</i>-caryophyllene ozonolysis products and mixtures with commercially available organic compounds journal October 2020
Effects of liquid–liquid phase separation and relative humidity on the heterogeneous OH oxidation of inorganic–organic aerosols: insights from methylglutaric acid and ammonium sulfate particles journal February 2021

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