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Published May 12, 2010 | Published + Supplemental Material
Journal Article Open

A global perspective on aerosol from low-volatility organic compounds


Global production of organic aerosol from primary emissions of semivolatile (SVOCs) and intermediate (IVOCs) volatility organic compounds is estimated using the global chemical transport model, GEOS-Chem. SVOC oxidation is predicted to be a larger global source of net aerosol production than oxidation of traditional parent hydrocarbons (terpenes, isoprene, and aromatics). Using a prescribed rate constant and reduction in volatility for atmospheric oxidation, the yield of aerosol from SVOCs is predicted to be about 75% on a global, annually-averaged basis. For IVOCs, the use of a naphthalene-like surrogate with different high-NOx and low-NOx parameterizations produces a global aerosol yield of about 30%, or roughly 5 Tg/yr of aerosol. Estimates of the total global organic aerosol source presented here range between 60 and 100 Tg/yr. This range reflects uncertainty in the parameters for SVOC volatility, SVOC oxidation, SVOC emissions, and IVOC emissions, as well as wet deposition. The highest estimates result if SVOC emissions are significantly underestimated (by more than a factor of 2) or if wet deposition of the gas-phase semivolatile species is less effective than previous estimates. A significant increase in SVOC emissions, a reduction of the volatility of the SVOC emissions, or an increase in the enthalpy of vaporization of the organic aerosol all lead to an appreciable reduction of prediction/measurement discrepancy. In addition, if current primary organic aerosol (POA) inventories capture only about one-half of the SVOC emission and the Henrys Law coefficient for oxidized semivolatiles is on the order of 10^3 M/atm, a global estimate of OA production is not inconsistent with the top-down estimate of 140 Tg/yr by (Goldstein and Galbally, 2007). Additional information is needed to constrain the emissions and treatment of SVOCs and IVOCs, which have traditionally not been included in models.

Additional Information

© 2010 Author(s). This work is distributed under the Creative Commons Attribution 3.0 License. Received: 21 January 2010; Published in Atmos. Chem. Phys. Discuss.: 11 February 2010; Revised: 28 April 2010; Accepted: 2 May 2010; Published: 12 May 2010. The numerical simulations for this research were performed on Caltech's Division of Geological and Planetary Sciences Dell cluster. H. O. T. P. acknowledges support by a National Science Foundation Graduate Research Fellowship. This research has been supported by the US Environmental Protection Agency Science to Achieve Results (STAR) agreements RD-833749 and RD-83337001 and by the Office of Science (BER), US Department of Energy Grant No. DE-FG02-05ER63983. Although the research described in the article has been funded in part by the US Environmental Protection Agency's STAR program, it has not been subjected to any EPA review and therefore does not necessarily reflect the views of the Agency, and no official endorsement should be inferred. The authors would like to thank Arthur Chan, Jose Jimenez, Fabien Paulot, and Paul Wennberg for useful discussions. Edited by: M. Kanakidou

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Published - Pye2010p10167Atmos_Chem_Phys.pdf

Supplemental Material - acp-10-4377-2010-supplement.pdf


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