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Issue 4, 2012
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The statistical evolution of multiple generations of oxidation products in the photochemical aging of chemically reduced organic aerosol

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Abstract

The heterogeneous reactions of hydroxyl radicals (OH) with squalane and bis(2-ethylhexyl) sebacate (BES) particles are used as model systems to examine how distributions of reaction products evolve during the oxidation of chemically reduced organic aerosol. A kinetic model of multigenerational chemistry, which is compared to previously measured (squalane) and new (BES) experimental data, reveals that it is the statistical mixtures of different generations of oxidation products that control the average particle mass and elemental composition during the reaction. The model suggests that more highly oxidized reaction products, although initially formed with low probability, play a large role in the production of gas phase reaction products. In general, these results highlight the importance of considering atmospheric oxidation as a statistical process, further suggesting that the underlying distribution of molecules could play important roles in aerosol formation as well as in the evolution of key physicochemical properties such as volatility and hygroscopicity.

Graphical abstract: The statistical evolution of multiple generations of oxidation products in the photochemical aging of chemically reduced organic aerosol

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Article information


Submitted
24 Aug 2011
Accepted
21 Nov 2011
First published
12 Dec 2011

Phys. Chem. Chem. Phys., 2012,14, 1468-1479
Article type
Paper

The statistical evolution of multiple generations of oxidation products in the photochemical aging of chemically reduced organic aerosol

K. R. Wilson, J. D. Smith, S. H. Kessler and J. H. Kroll, Phys. Chem. Chem. Phys., 2012, 14, 1468
DOI: 10.1039/C1CP22716E

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