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| Titel |
Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: evaluation of the volatility-basis-set approach within the CHIMERE model |
| VerfasserIn |
Q. J. Zhang, M. Beekmann, F. Drewnick, F. Freutel, J. Schneider, M. Crippa, A. S. H. Prévôt, U. Baltensperger, L. Poulain, A. Wiedensohler, J. Sciare, V. Gros, A. Borbon, A. Colomb, V. Michoud, J.-F. Doussin, H. A. C. Denier van der Gon, M. Haeffelin, J.-C. Dupont, G. Siour, H. Petetin, B. Bessagnet, S. N. Pandis, A. Hodzic, O. Sanchez, C. Honore, O. Perrussel |
| 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 ; 13, no. 11 ; Nr. 13, no. 11 (2013-06-14), S.5767-5790 |
| Datensatznummer |
250018703
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| Publikation (Nr.) |
 copernicus.org/acp-13-5767-2013.pdf |
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| Zusammenfassung |
| Simulations with the chemistry transport model CHIMERE
are compared to measurements performed during the MEGAPOLI
(Megacities: Emissions, urban, regional and Global Atmospheric
POLlution and climate effects, and Integrated tools for assessment and
mitigation) summer campaign
in the Greater Paris region in July 2009. The volatility-basis-set approach
(VBS) is implemented into this model, taking into account the volatility of
primary organic aerosol (POA) and the chemical aging of semi-volatile
organic species. Organic aerosol is the main focus and is simulated with
three different configurations with a modified treatment of POA volatility
and modified secondary organic aerosol (SOA) formation schemes. In addition,
two types of emission inventories are used as model input in order to test
the uncertainty related to the emissions. Predictions of basic
meteorological parameters and primary and secondary pollutant concentrations
are evaluated, and four pollution regimes are defined according to the air mass
origin. Primary pollutants are generally overestimated, while ozone is
consistent with observations. Sulfate is generally overestimated, while
ammonium and nitrate levels are well simulated with the refined emission
data set. As expected, the simulation with non-volatile POA and a
single-step SOA formation mechanism largely overestimates POA and
underestimates SOA. Simulation of organic aerosol with the VBS approach
taking into account the aging of semi-volatile organic compounds (SVOC)
shows the best correlation with measurements. High-concentration events
observed mostly after long-range transport are well reproduced by the model.
Depending on the emission inventory used, simulated POA levels are either
reasonable or underestimated, while SOA levels tend to be overestimated.
Several uncertainties related to the VBS scheme (POA volatility, SOA yields,
the aging parameterization), to emission input data, and to simulated OH
levels can be responsible for this behavior. Despite these uncertainties,
the implementation of the VBS scheme into the CHIMERE model allowed for much
more realistic organic aerosol simulations for Paris during summertime. The
advection of SOA from outside Paris is mostly responsible for the highest OA
concentration levels. During advection of polluted air masses from
northeast (Benelux and Central Europe), simulations indicate high levels of
both anthropogenic and biogenic SOA fractions, while biogenic SOA dominates
during periods with advection from Southern France and Spain. |
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