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Dynamics of Liquid-Liquid Phase Separation in Submicrometer Aerosol
Theresa M Kucinski1, Emily-Jean E Ott1, Miriam Arak Freedman1
1Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States.
The Journal of Physical Chemistry. A
|May 17, 2021
Summary
Submicrometer aerosol particles exhibit lower phase separation conditions than larger droplets. This finding suggests current climate models may overestimate phase-separated aerosols, necessitating updated representations of aerosol phase transitions.
Area of Science:
- Atmospheric Chemistry
- Materials Science
- Physical Chemistry
Background:
- Nanoscale materials exhibit unique properties distinct from their bulk counterparts.
- Liquid-liquid phase separation (LLPS) is a critical phenomenon in atmospheric aerosols, influencing their properties and climate impact.
- LLPS in aerosols is typically studied as a function of water activity, equivalent to relative humidity (RH).
Purpose of the Study:
- To investigate the influence of particle size on the conditions of liquid-liquid phase separation (LLPS) in organic/inorganic aerosol systems.
- To compare the phase separation relative humidity (SRH) of submicrometer aerosol particles with micrometer-sized droplets.
- To assess the implications of nanoscale phase behavior for climate modeling and aerosol characterization.
Main Methods:
- Experimental probing of three organic/inorganic aerosol systems.
- Measurement of phase separation relative humidity (SRH) across a range of relative humidity conditions.
- Comparison of SRH values for submicrometer particles versus micrometer-sized droplets.
Main Results:
- The study found that the SRH for submicrometer aerosol particles is lower compared to micrometer-sized droplets.
- This size-dependent shift in phase separation conditions was observed across the investigated organic/inorganic aerosol systems.
- The findings indicate a potential overestimation of phase-separated aerosols in current climate models.
Conclusions:
- The representation of phase transitions in atmospheric aerosol particles within climate models may require updates to account for nanoscale effects.
- A decrease in SRH for submicrometer particles suggests that a larger fraction of atmospheric aerosols may be phase-separated than currently estimated.
- Understanding LLPS at the nanoscale is crucial for accurate aerosol characterization and improved climate predictions.

