Variations in organic aerosol optical and hygroscopic properties upon heterogeneous OH oxidation
Measurements of the evolution of organic aerosol extinction cross sections (σext) and subsaturated hygroscopicity upon heterogeneous OH oxidation are reported for two model compounds, squalane (a C30 saturated hydrocarbon) and azelaic acid (a C9 dicarboxylic acid). For both compounds, the σext value...
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| Published in | Journal of Geophysical Research Vol. 116; no. D15 |
|---|---|
| Main Authors | , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Washington
Blackwell Publishing Ltd
06.08.2011
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Measurements of the evolution of organic aerosol extinction cross sections (σext) and subsaturated hygroscopicity upon heterogeneous OH oxidation are reported for two model compounds, squalane (a C30 saturated hydrocarbon) and azelaic acid (a C9 dicarboxylic acid). For both compounds, the σext values at 532 nm increase substantially as the particles undergo oxidation, exhibiting a logarithmic increase with OH exposure. The increase in σext correlates with both an increase in the particle oxygen to carbon (O:C) atomic ratio and density and a decrease in mean molecular weight. The measurements have been used to calculate the variation with oxidation of the mean polarizability, α, of the molecules comprising the particles. The absolute α values for the two systems are shown to be related through the variation in the particle chemical composition, specifically the relative abundances of C, O, and H atoms and the mean molecular weight. Unlike σext, it was found that the evolution of the particle hygroscopicity upon oxidation is quite different for the two model systems considered. Hygroscopicity was quantified by measuring γext, which is a single‐parameter representation of hygroscopicity that describes the increase in extinction upon exposure of the particles to a high–relative humidity environment (here, 75% and 85% RH). For unoxidized squalane, γext was zero and only increased slowly as the particles were oxidized by OH radicals. In contrast, γext for azelaic acid increased rapidly upon exposure to OH, eventually reaching a plateau at high OH exposures. In general, γext appears to vary sigmoidally with O:C, reaching a plateau at high O:C.
Key Points
Organic aerosol optical properties are not static
Organic aerosol optical properties are directly related to the mean composition
OA hygroscopicity depends on both atomic composition and molecular volume |
|---|---|
| AbstractList | Organic aerosol optical properties are not static Organic aerosol optical properties are directly related to the mean composition OA hygroscopicity depends on both atomic composition and molecular volume Measurements of the evolution of organic aerosol extinction cross sections (ext) and subsaturated hygroscopicity upon heterogeneous OH oxidation are reported for two model compounds, squalane (a C30 saturated hydrocarbon) and azelaic acid (a C9 dicarboxylic acid). For both compounds, the ext values at 532 nm increase substantially as the particles undergo oxidation, exhibiting a logarithmic increase with OH exposure. The increase in ext correlates with both an increase in the particle oxygen to carbon (O:C) atomic ratio and density and a decrease in mean molecular weight. The measurements have been used to calculate the variation with oxidation of the mean polarizability, , of the molecules comprising the particles. The absolute values for the two systems are shown to be related through the variation in the particle chemical composition, specifically the relative abundances of C, O, and H atoms and the mean molecular weight. Unlike ext, it was found that the evolution of the particle hygroscopicity upon oxidation is quite different for the two model systems considered. Hygroscopicity was quantified by measuring ext, which is a single-parameter representation of hygroscopicity that describes the increase in extinction upon exposure of the particles to a highrelative humidity environment (here, 75% and 85% RH). For unoxidized squalane, ext was zero and only increased slowly as the particles were oxidized by OH radicals. In contrast, ext for azelaic acid increased rapidly upon exposure to OH, eventually reaching a plateau at high OH exposures. In general, ext appears to vary sigmoidally with O:C, reaching a plateau at high O:C. Measurements of the evolution of organic aerosol extinction cross sections (σext) and subsaturated hygroscopicity upon heterogeneous OH oxidation are reported for two model compounds, squalane (a C30 saturated hydrocarbon) and azelaic acid (a C9 dicarboxylic acid). For both compounds, the σext values at 532 nm increase substantially as the particles undergo oxidation, exhibiting a logarithmic increase with OH exposure. The increase in σext correlates with both an increase in the particle oxygen to carbon (O:C) atomic ratio and density and a decrease in mean molecular weight. The measurements have been used to calculate the variation with oxidation of the mean polarizability, α, of the molecules comprising the particles. The absolute α values for the two systems are shown to be related through the variation in the particle chemical composition, specifically the relative abundances of C, O, and H atoms and the mean molecular weight. Unlike σext, it was found that the evolution of the particle hygroscopicity upon oxidation is quite different for the two model systems considered. Hygroscopicity was quantified by measuring γext, which is a single‐parameter representation of hygroscopicity that describes the increase in extinction upon exposure of the particles to a high–relative humidity environment (here, 75% and 85% RH). For unoxidized squalane, γext was zero and only increased slowly as the particles were oxidized by OH radicals. In contrast, γext for azelaic acid increased rapidly upon exposure to OH, eventually reaching a plateau at high OH exposures. In general, γext appears to vary sigmoidally with O:C, reaching a plateau at high O:C. Key Points Organic aerosol optical properties are not static Organic aerosol optical properties are directly related to the mean composition OA hygroscopicity depends on both atomic composition and molecular volume Organic aerosol optical properties are not static Organic aerosol optical properties are directly related to the mean composition OA hygroscopicity depends on both atomic composition and molecular volume Measurements of the evolution of organic aerosol extinction cross sections ( sigma ext) and subsaturated hygroscopicity upon heterogeneous OH oxidation are reported for two model compounds, squalane (a C30 saturated hydrocarbon) and azelaic acid (a C9 dicarboxylic acid). For both compounds, the sigma ext values at 532 nm increase substantially as the particles undergo oxidation, exhibiting a logarithmic increase with OH exposure. The increase in sigma ext correlates with both an increase in the particle oxygen to carbon (O:C) atomic ratio and density and a decrease in mean molecular weight. The measurements have been used to calculate the variation with oxidation of the mean polarizability, alpha , of the molecules comprising the particles. The absolute alpha values for the two systems are shown to be related through the variation in the particle chemical composition, specifically the relative abundances of C, O, and H atoms and the mean molecular weight. Unlike sigma ext, it was found that the evolution of the particle hygroscopicity upon oxidation is quite different for the two model systems considered. Hygroscopicity was quantified by measuring gamma ext, which is a single-parameter representation of hygroscopicity that describes the increase in extinction upon exposure of the particles to a high-relative humidity environment (here, 75% and 85% RH). For unoxidized squalane, gamma ext was zero and only increased slowly as the particles were oxidized by OH radicals. In contrast, gamma ext for azelaic acid increased rapidly upon exposure to OH, eventually reaching a plateau at high OH exposures. In general, gamma ext appears to vary sigmoidally with O:C, reaching a plateau at high O:C. |
| ArticleNumber | D15204 |
| Author | Kroll, Jesse H. Che, Daphne L. Wilson, Kevin R. Cappa, Christopher D. Kessler, Sean H. |
| Author_xml | – sequence: 1 givenname: Christopher D. surname: Cappa fullname: Cappa, Christopher D. email: cdcappa@ucdavis.edu organization: Department of Civil and Environmental Engineering, University of California, California, Davis, USA – sequence: 2 givenname: Daphne L. surname: Che fullname: Che, Daphne L. organization: Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, USA – sequence: 3 givenname: Sean H. surname: Kessler fullname: Kessler, Sean H. organization: Department of Chemical Engineering, Massachusetts Institute of Technology, Massachusetts, Cambridge, USA – sequence: 4 givenname: Jesse H. surname: Kroll fullname: Kroll, Jesse H. organization: Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts, USA – sequence: 5 givenname: Kevin R. surname: Wilson fullname: Wilson, Kevin R. organization: Chemical Sciences Division, Lawrence Berkeley National Laboratory, California, Berkeley, USA |
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| Snippet | Measurements of the evolution of organic aerosol extinction cross sections (σext) and subsaturated hygroscopicity upon heterogeneous OH oxidation are reported... Organic aerosol optical properties are not static Organic aerosol optical properties are directly related to the mean composition OA hygroscopicity depends on... |
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| SubjectTerms | Aerosols Atmospheric aerosols Atmospheric sciences Geophysics Hygroscopicity Optical Properties Organic Aerosol Oxidation Saturated hydrocarbons |
| Title | Variations in organic aerosol optical and hygroscopic properties upon heterogeneous OH oxidation |
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