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Biogenic SOA formation through gas-phase oxidation and gas-to-particle partitioning-a comparison between process models of varying complexity

Öström, Emilie LU ; Roldin, Pontus LU ; Rusanen, A.; Mogensen, D.; Kivekäs, Niku LU ; Väänänen, R.; Boy, M. and Swietlicki, Erik LU (2014) In Atmospheric Chemistry and Physics 14(21). p.11853-11869
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... (More)
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. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Atmospheric Chemistry and Physics
volume
14
issue
21
pages
11853 - 11869
publisher
Copernicus Gesellschaft Mbh
external identifiers
  • wos:000344985700018
  • scopus:84909592065
ISSN
1680-7324
DOI
10.5194/acp-14-11853-2014
project
MERGE
language
English
LU publication?
yes
id
427d76df-c140-4362-a98f-3cf16a4f7173 (old id 4857281)
date added to LUP
2014-12-05 14:05:43
date last changed
2017-08-06 03:17:54
@article{427d76df-c140-4362-a98f-3cf16a4f7173,
  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.},
  author       = {Öström, Emilie and Roldin, Pontus and Rusanen, A. and Mogensen, D. and Kivekäs, Niku and Väänänen, R. and Boy, M. and Swietlicki, Erik},
  issn         = {1680-7324},
  language     = {eng},
  number       = {21},
  pages        = {11853--11869},
  publisher    = {Copernicus Gesellschaft Mbh},
  series       = {Atmospheric Chemistry and Physics},
  title        = {Biogenic SOA formation through gas-phase oxidation and gas-to-particle partitioning-a comparison between process models of varying complexity},
  url          = {http://dx.doi.org/10.5194/acp-14-11853-2014},
  volume       = {14},
  year         = {2014},
}