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Title: Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state: CLOUD ACTIVATION BY AGED ORGANIC AEROSOL

Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation of liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.
Authors:
 [1] ; ORCiD logo [2] ;  [3] ; ORCiD logo [4] ;  [3] ;  [5] ; ORCiD logo [6]
  1. Stony Brook University, Institute for Terrestrial and Planetary Atmospheres, School of Marine and Atmospheric Sciences, Stony Brook NY USA; Now at Purdue University, Department of Chemistry, West Lafayette IN USA
  2. Max Planck Institute for Chemistry, Multiphase Chemistry Department, Mainz Germany; University of California, Irvine, Department of Chemistry, Irvine CA USA
  3. Max Planck Institute for Chemistry, Multiphase Chemistry Department, Mainz Germany
  4. Max Planck Institute for Chemistry, Multiphase Chemistry Department, Mainz Germany; Institute for Environmental and Climate Research, Jinan University, Guangzhou China
  5. Brookhaven National Laboratory, Environmental and Climate Sciences Department, Upton NY USA
  6. Stony Brook University, Institute for Terrestrial and Planetary Atmospheres, School of Marine and Atmospheric Sciences, Stony Brook NY USA
Publication Date:
Report Number(s):
BNL-113518-2017-JA
Journal ID: ISSN 0094-8276; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000
Grant/Contract Number:
SC0012704; AGS-0846255; AGS-1446286; AC02098CH10886
Type:
Accepted Manuscript
Journal Name:
Geophysical Research Letters
Additional Journal Information:
Journal Volume: 44; Journal Issue: 3; Journal ID: ISSN 0094-8276
Publisher:
American Geophysical Union
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); National Science Foundation (NSF); European Union (EU); Max Planck Society
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; organic aerosol; chemical aging; viscosity; cloud formation; hygroscopicity; OH oxidation
OSTI Identifier:
1344233