ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-11-1083-2011 A secondary organic aerosol formation model considering successive oxidation aging and kinetic condensation of organic compounds: global scale implications Yu F. 1 Atmospheric Sciences Research Center, State University of New York, Albany, New York, USA 08 02 2011 11 3 1083 1099 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/11/1083/2011/acp-11-1083-2011.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/1083/2011/acp-11-1083-2011.pdf

The widely used two-product secondary organic aerosol (SOA) formation model has been extended in this study to consider the volatility changes of secondary organic gases (SOG) arising from the aging process as well as the kinetic condensation of low volatile SOG (LV-SOG). In addition to semi-volatile SOG (SV-SOG) with saturation vapor pressure at 290 K (<i>C</i><sup>*</sup><sub>290</sub>) in the range of ~3 ppt–3 ppb and medium-volatile SOG (MV-SOG) with <i>C</i><sup>*</sup><sub>290</sub> in the range of ~0.3–300 ppb, we add a third component representing LV-SOG with <i>C</i><sup>*</sup><sub>290</sub> below ~3 ppt and design a scheme to transfer MV-SOG to SV-SOG and SV-SOG to LV-SOG associated with oxidation aging. This extended SOA formation model has been implemented in a global aerosol model (GEOS-Chem) and the co-condensation of H<sub>2</sub>SO<sub>4</sub> and LV-SOG on pre-existing particles is explicitly simulated. We show that, over many parts of the continents, LV-SOG concentrations are generally a factor of ~2–20 higher than those of H<sub>2</sub>SO<sub>4</sub> and the kinetic condensation of LV-SOG significantly enhances particle growth rates. Comparisons of the simulated and observed evolution of particle size distributions at a boreal forest site (Hyytiälä, Finland) clearly show that LV-SOG condensation is critical in order to bring the simulations closer to the observations. With the new SOA formation scheme, annual mean SOA mass increases by a factor of 2–10 in many parts of the boundary layer and reaches above 0.5 μg m<sup>−3</sup> in most parts of the main continents, improving the agreement with aerosol mass spectrometer (AMS) SOA measurements. While the new scheme generally decreases the concentration of condensation nuclei larger than 10 nm by 3–30% in the lower boundary layer as a result of enhanced surface area and reduced nucleation rates, it substantially increases the concentration of cloud condensation nuclei at a water supersaturation ratio of 0.2%, ranging from ~5–20% over a large fraction of oceans and high latitude continents to more than 50% over some parts of South America, Australia, and Indonesia. Our study highlights the importance for global aerosol models to explicitly account for the oxidation aging of SOGs and their contribution to particle growth.

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