Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity

Thalman, R.; Thalman, R.; Wang, J.; Knopf, D. A.

doi:10.5194/acpd-15-6771-2015

Title: Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: Implications for cloud condensation nucleus activity

Journal Article · Fri Mar 06 00:00:00 EST 2015 · Atmospheric Chemistry and Physics Discussions (Online)

DOI:https://doi.org/10.5194/acpd-15-6771-2015· OSTI ID:1190765

Thalman, R. ^[1]; Thalman, R. ^[2]; Wang, J. ^[2]; Knopf, D. A. ^[1]

State Univ. of New York (SUNY), Stony Brook, NY (United States). School of Marine and Atmospheric Sciences.
Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Environmental and Climate Sciences.

Multiphase OH and O₃ oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O₃ can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O₃ is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O₃ exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O₃ exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1:1 by mass MNC: KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging has no significant impact on OA hygroscopicity. The organic compounds exhibiting low solubility behave as if they are infinitely soluble when mixed with a sufficient amount of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and not influenced by the oxidized organic fraction. Our results have important implications for heterogeneous oxidation and its impact on cloud formation given that atmospheric aerosol is a complex mixture of organic and inorganic compounds exhibiting a wide-range of solubilities.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC00112704

OSTI ID:: 1190765

Report Number(s):: BNL-107841-2015-JA; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000

Journal Information:: Atmospheric Chemistry and Physics Discussions (Online), Vol. 15, Issue 5; ISSN 1680-7375

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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