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Titel |
Secondary organic aerosol formation during June 2010 in Central Europe: measurements and modelling studies with a mixed thermodynamic-kinetic approach |
VerfasserIn |
B. Langmann, K. Sellegri, E. Freney |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 14, no. 8 ; Nr. 14, no. 8 (2014-04-16), S.3831-3842 |
Datensatznummer |
250118619
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Publikation (Nr.) |
copernicus.org/acp-14-3831-2014.pdf |
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Zusammenfassung |
Until recently secondary organic carbon aerosol (SOA) mass concentrations
have been systematically underestimated by three-dimensional
atmospheric-chemistry-aerosol models. With a newly proposed concept of aging
of organic vapours, more realistic model results for organic carbon aerosol
mass concentrations can be achieved. Applying a mixed thermodynamic-kinetic
approach for SOA formation shifted the aerosol size distribution towards
particles in the cloud condensation nuclei size range, thereby emphasising
the importance of SOA formation schemes for modelling realistic cloud and
precipitation formation. The additional importance of hetero-molecular
nucleation between H2SO4 and organic vapours remains to be
evaluated in three-dimensional atmospheric-chemistry-aerosol models. Here a
case study is presented focusing on Puy-de-Dôme, France in June 2010.
The measurements indicate a considerable increase in SOA mass concentration
during the measurement campaign, which could be reproduced by modelling
using a simplified thermodynamic-kinetic approach for SOA formation and
increased biogenic volatile organic compound (VOC) precursor emissions. Comparison with a thermodynamic
SOA formation approach shows a huge improvement in modelled SOA mass
concentration with the thermodynamic-kinetic approach for SOA formation. SOA
mass concentration increases by a factor of up to 6 accompanied by a slight
improvement of modelled particle size distribution. Even though nucleation
events at Puy-de-Dôme were rare during the chosen period of
investigation, a weak event in the boundary layer could be reproduced by the
model in a sensitivity study when nucleation of low-volatile secondary
organic vapour is included. Differences in the model results with and
without nucleation of organic vapour are visible in the lower free
troposphere over several days. Taking into account the nucleation of organic
vapour leads to an increase in accumulation mode particles due to
coagulation and condensational growth of nucleation and Aitken mode
particles. |
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