Atmospheric Chemistry and Physics Discussions
www.atmos-chem-phys-discuss.net
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7
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2007
10.5194/acpd-7-8951-2007
http://www.atmos-chem-phys-discuss.net/7/8951/2007/
http://www.atmos-chem-phys-discuss.net/7/8951/2007/acpd-7-8951-2007.html
http://www.atmos-chem-phys-discuss.net/7/8951/2007/acpd-7-8951-2007.pdf
8951
8982
2007-06-26
Modeling secondary organic aerosol formation through cloud processing of organic compounds
J. Chen
jianjunc@cisunix.unh.edu
R. J. Griffin
A. Grini
P. Tulet
Institute for the Study of Earth, Oceans, and Space, University of New Hampshire, Durham, NH, USA
Department of Earth Sciences, University of New Hampshire, Durham, NH, USA
Department of Geoscience, University of Oslo, Pb 1022 Blindern, 0315, Oslo, Norway
CNRM/GMEI Météo France, Toulouse, France
Interest in the potential formation of secondary organic aerosol (SOA)
through reactions of organic compounds in condensed aqueous phases is
growing. In this study, the potential formation of SOA from irreversible
aqueous-phase reactions of organic species in clouds was investigated. A new
proposed aqueous-phase chemistry mechanism (AqChem) is coupled with the
existing gas-phase Caltech Atmospheric Chemistry Mechanism (CACM) and the
Model to Predict the Multiphase Partitioning of Organics (MPMPO) that
simulate SOA formation. AqChem treats irreversible organic reactions that
lead mainly to the formation of carboxylic acids, which are usually less
volatile than the corresponding aldehydic compounds. Zero-dimensional model
simulations were performed for tropospheric conditions with clouds present
for three consecutive hours per day. Zero-dimensional model simulations show
that 48-h averaged SOA formation are increased by 27% for a rural
scenario with strong monoterpene emissions and 7% for an urban scenario
with strong emissions of aromatic compounds, respectively, when irreversible
organic reactions in clouds are considered. AqChem was also incorporated
into the Community Multiscale Air Quality Model (CMAQ) version 4.4 with
CACM/MPMPO and applied to a previously studied photochemical episode (3–4 August 2004) focusing on the eastern United States. The CMAQ study indicates
that the maximum contribution of SOA formation from irreversible reactions
of organics in clouds is 0.28 μg m<sup>−3</sup> for 24-h average
concentrations and 0.60 μg m<sup>−3</sup> for one-hour average concentrations
at certain locations. On average, domain-wide surface SOA predictions for
the episode are increased by 8.6% when irreversible, in-cloud processing
of organics is considered.
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