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Title: The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review

Abstract

Predicting the formation of ice crystals in the atmosphere presents one of the great challenges in physical sciences with important implications for the chemistry and composition of the Earth’s atmosphere, the hydrological cycle, and climate. Among atmospheric ice formation processes, heterogeneous ice nucleation proceeds on aerosol particles ranging from a few nanometers to micrometers in size, commonly referred to as ice nucleating particles (INPs). Research over the last two decades has demonstrated that organic matter (OM) is ubiquitous in the atmosphere, present as organic aerosol (OA) particles or as coatings on other particle types. While it is well understood that mineral dust particles can induce ice nucleation under atmospheric conditions, it is currently not clear how much OA particles including pollution aerosol and secondary organic aerosol (SOA) contributes to the ambient INP population. The physicochemical properties of OM make predicting how OM interacts with water vapor leading ultimately to ice crystals challenging. This review focuses on the role of OM in INPs, summarizing and highlighting recent advances in our understanding of the ice nucleation process gained from theoretical, laboratory, and field studies. Examination of ice residuals and INPs with analytical techniques demonstrates that OM participates in atmospheric ice crystal formation.more » Molecular dynamic simulations provide insight into the microscopic processes that initiate ice nucleation. The amorphous phase state of OM in the supercooled and metastable regime is identified as a key factor in assessing the particles’ nucleation pathways and rates. A theoretical model is advanced, based on particle water activity, to holistically predict amorphous phase changes and ice nucleation rates of particles coated by OM. The goal of this review is to synthesize our current understanding and propose future research directions needed to fully evaluate how OA particles contribute to INPs in the atmosphere.« less

Authors:
ORCiD logo [1];  [2];  [3]
  1. Stony Brook Univ., NY (United States)
  2. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  3. Xiamen Univ. (China)
Publication Date:
Research Org.:
Stony Brook Univ., NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1498735
Grant/Contract Number:  
SC0016370
Resource Type:
Accepted Manuscript
Journal Name:
ACS Earth and Space Chemistry
Additional Journal Information:
Journal Volume: 2; Journal Issue: 3; Journal ID: ISSN 2472-3452
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; organic aerosol; ice nucleation; organic matter; amorphous phase state; molecular dynamics simulation; laboratory experiments; field measurements; organic coating

Citation Formats

Knopf, Daniel A., Alpert, Peter A., and Wang, Bingbing. The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review. United States: N. p., 2018. Web. doi:10.1021/acsearthspacechem.7b00120.
Knopf, Daniel A., Alpert, Peter A., & Wang, Bingbing. The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review. United States. doi:10.1021/acsearthspacechem.7b00120.
Knopf, Daniel A., Alpert, Peter A., and Wang, Bingbing. Fri . "The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review". United States. doi:10.1021/acsearthspacechem.7b00120. https://www.osti.gov/servlets/purl/1498735.
@article{osti_1498735,
title = {The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review},
author = {Knopf, Daniel A. and Alpert, Peter A. and Wang, Bingbing},
abstractNote = {Predicting the formation of ice crystals in the atmosphere presents one of the great challenges in physical sciences with important implications for the chemistry and composition of the Earth’s atmosphere, the hydrological cycle, and climate. Among atmospheric ice formation processes, heterogeneous ice nucleation proceeds on aerosol particles ranging from a few nanometers to micrometers in size, commonly referred to as ice nucleating particles (INPs). Research over the last two decades has demonstrated that organic matter (OM) is ubiquitous in the atmosphere, present as organic aerosol (OA) particles or as coatings on other particle types. While it is well understood that mineral dust particles can induce ice nucleation under atmospheric conditions, it is currently not clear how much OA particles including pollution aerosol and secondary organic aerosol (SOA) contributes to the ambient INP population. The physicochemical properties of OM make predicting how OM interacts with water vapor leading ultimately to ice crystals challenging. This review focuses on the role of OM in INPs, summarizing and highlighting recent advances in our understanding of the ice nucleation process gained from theoretical, laboratory, and field studies. Examination of ice residuals and INPs with analytical techniques demonstrates that OM participates in atmospheric ice crystal formation. Molecular dynamic simulations provide insight into the microscopic processes that initiate ice nucleation. The amorphous phase state of OM in the supercooled and metastable regime is identified as a key factor in assessing the particles’ nucleation pathways and rates. A theoretical model is advanced, based on particle water activity, to holistically predict amorphous phase changes and ice nucleation rates of particles coated by OM. The goal of this review is to synthesize our current understanding and propose future research directions needed to fully evaluate how OA particles contribute to INPs in the atmosphere.},
doi = {10.1021/acsearthspacechem.7b00120},
journal = {ACS Earth and Space Chemistry},
number = 3,
volume = 2,
place = {United States},
year = {2018},
month = {1}
}

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