Journal cover Journal topic
Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
Atmos. Chem. Phys., 14, 11853-11869, 2014
http://www.atmos-chem-phys.net/14/11853/2014/
doi:10.5194/acp-14-11853-2014
© Author(s) 2014. This work is distributed
under the Creative Commons Attribution 3.0 License.
Research article
12 Nov 2014
Biogenic SOA formation through gas-phase oxidation and gas-to-particle partitioning – a comparison between process models of varying complexity
E. Hermansson1,2, P. Roldin1,3, A. Rusanen3, D. Mogensen3, N. Kivekäs1,*, R. Väänänen3, M. Boy3, and E. Swietlicki1,2 1Division of Nuclear Physics, Lund University, P.O. Box 118, 221 00, Lund, Sweden
2Centre for Environmental and Climate Research, Lund University, P.O. Box 118, 221 00, Lund, Sweden
3Department of Physics, P.O. Box 64, 00014 University of Helsinki, Helsinki, Finland
*now at: Atmospheric Composition, Finnish Meteorological Institute, P.O. Box 503, 00101, Helsinki, Finland
Abstract. Biogenic volatile organic compounds (BVOCs) emitted by vegetation play an important role for aerosol mass loadings since the oxidation products of these compounds can take part in the formation and growth of secondary organic aerosols (SOA). The concentrations and properties of BVOCs and their oxidation products in the atmosphere are poorly characterized, which leads to high uncertainties in modeled SOA mass and properties. In this study, the formation of SOA has been modeled along an air-mass trajectory over northern European boreal forest using two aerosol dynamics box models where the prediction of the condensable organics from the gas-phase oxidation of BVOC is handled with schemes of varying complexity. The use of box model simulations along an air-mass trajectory allows us to compare, under atmospheric relevant conditions, different model parameterizations and their effect on SOA formation. The result of the study shows that the modeled mass concentration of SOA is highly dependent on the organic oxidation scheme used to predict oxidation products. A near-explicit treatment of organic gas-phase oxidation (Master Chemical Mechanism version 3.2) was compared to oxidation schemes that use the volatility basis set (VBS) approach. The resulting SOA mass modeled with different VBS schemes varies by a factor of about 7 depending on how the first-generation oxidation products are parameterized and how they subsequently age (e.g., how fast the gas-phase oxidation products react with the OH radical, how they respond to temperature changes, and if they are allowed to fragment during the aging process). Since the VBS approach is frequently used in regional and global climate models due to its relatively simple treatment of the oxidation products compared to near-explicit oxidation schemes, a better understanding of the above-mentioned processes is needed. Based on the results of this study, fragmentation should be included in order to obtain a realistic SOA formation. Furthermore, compared to the most commonly used VBS schemes, the near-explicit method produces less – but more oxidized – SOA.

Citation: Hermansson, E., Roldin, P., Rusanen, A., Mogensen, D., Kivekäs, N., Väänänen, R., Boy, M., and Swietlicki, E.: Biogenic SOA formation through gas-phase oxidation and gas-to-particle partitioning – a comparison between process models of varying complexity, Atmos. Chem. Phys., 14, 11853-11869, doi:10.5194/acp-14-11853-2014, 2014.
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Short summary
Secondary organic aerosols (SOA), produced through oxidation processes, constitute a large part of the global organic aerosol load and affect the climate. We found that the modeled mass of SOA was highly dependent on how the oxidation processes were explained in models. The results indicated that it was especially important to get the volatility distribution of the products from the first oxidation step right and that fragmentation during the oxidation process played an important role.
Secondary organic aerosols (SOA), produced through oxidation processes, constitute a large part...
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