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Title: Experimental Determination of the Relationship Between Organic Aerosol Viscosity and Ice Nucleation at Upper Free Tropospheric Conditions

Journal Article · · Journal of Geophysical Research: Atmospheres
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]
  1. Department of Marine, Earth, and Atmospheric Sciences NC State University Raleigh NC USA
  2. Department of Atmospheric Science Colorado State University Fort Collins CO USA
  3. University of Colorado Boulder Boulder CO USA
  4. University of Colorado Boulder Boulder CO USA, Now at NOAA Chemical Sciences Laboratory Boulder CO USA

Abstract This work presents measurements of the ice nucleating ability of secondary organic material recorded between −40 and −70°C and relative humidity with respect to ice (RH ice ) between 150% and 220%. For a subset of systems, temperature and humidity dependence of particle viscosity as well as dry glass transition temperature were characterized using the dual tandem differential mobility analyzer method. Eleven unique monoterpene, sesquiterpene and aromatic precursors were used to generate secondary organic material (SOM) using either an oxidation flow reactor (OFR) or an environmental chamber (EC). For the SOM for which viscosity was measured, the particle glass transition temperatures varied between 6 and 23°C ( n  = 8). Measurements were performed to verify that increased relative humidity did not plasticize the particles below −10°C at residence times similar to those in the ice nucleation instrument. No heterogeneous ice nucleation was observed at the ∼0.5% onset threshold for any of the materials generated. The ice nucleation occurs by the freezing of SOM solution droplets consistent with homogeneous freezing indicating that they form an aqueous solution, or the SOM particles required water saturation to freeze, indicating that they were hydrophobic. Experiments exploring the influence of functional groups and mass loading did not reveal any obvious influence of particle chemistry or generation conditions on the results. Close structural matches between known organic ice nucleating particles as precursor or formed products did not yield materials that promoted freezing. These experiments suggest that heterogeneous ice formation of glassy secondary organic materials is likely uncommon under upper free tropospheric conditions.

Sponsoring Organization:
USDOE
Grant/Contract Number:
SC0018265
OSTI ID:
1881060
Journal Information:
Journal of Geophysical Research: Atmospheres, Journal Name: Journal of Geophysical Research: Atmospheres Journal Issue: 16 Vol. 127; ISSN 2169-897X
Publisher:
American Geophysical Union (AGU)Copyright Statement
Country of Publication:
United States
Language:
English

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