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Title: Images reveal that atmospheric particles can undergo liquid-liquid phase separations

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America

A large fraction of submicron atmospheric particles contains both organic material and inorganic salts. As the relative humidity cycles in the atmosphere, these mixed particles can undergo a range of phase transitions, possibly including liquid-liquid phase separation. If liquid-liquid phase separation occurs, the gas-particle partitioning of atmospheric semi-volatile organic compounds, the scattering and absorption of solar radiation, and the uptake of reactive gas species on atmospheric particles will be affected, with important implications for climate predictions. The actual occurrence of these types of phase transitions within individual atmospheric particles has been considered uncertain, in large part because of the absence of observations for real-world samples. Here, using optical and fluorescence microscopy, we observe the coexistence of two non-crystalline phases in particles generated from real-world samples collected on multiple days in Atlanta, Georgia, and in particles generated in the laboratory using atmospheric conditions. These results reveal that atmospheric particles can undergo liquid-liquid phase separations. Using a box model, we show that liquid-liquid phase separation can result in increased concentrations of gas-phase NO3 and N2O5 in the Atlanta region, due to decreased particle uptake of N2O5.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1049026
Report Number(s):
PNNL-SA-85901; PNASA6; TRN: US201217%%297
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 109, Issue 33; ISSN 0027-8424
Country of Publication:
United States
Language:
English

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