Atmos. Chem. Phys. Discuss., 12, 29475-29533, 2012
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: evaluation of the Volatility-Basis-Set approach within the CHIMERE model
Q. J. Zhang1,13, M. Beekmann1, F. Drewnick2, F. Freutel2, J. Schneider2, M. Crippa3, A. S. H. Prévôt1, U. Baltensperger3, L. Poulain4, A. Wiedensohler4, J. Sciare5, V. Gros5, A. Borbon1, A. Colomb1,6, V. Michoud1, J.-F. Doussin1, H. A. C. Denier van der Gon7, M. Haeffelin8, J.-C. Dupont8, G. Siour1,9, H. Petetin1,12, B. Bessagnet9, S. N. Pandis10, A. Hodzic11, O. Sanchez12, C. Honoré12, and O. Perrussel12
1LISA/IPSL, Laboratoire Interuniversitaire des Systèmes Atmosphériques, CNRS, UMR7583, Université Paris Est Créteil (UPEC) et Université Paris Diderot (UPD), Créteil, France
2Max Planck Institute for Chemistry, Particle Chemistry Department, Mainz, Germany
3Paul Scherrer Institute, Villigen, Switzerland
4Leibniz Institute for Troposphärenforschung, Leipzig, Germany
5Laboratoire des sciences du climat et de l'environnement, IPSL, CEA et l'Université de Versailles, CNRS, Saint-Quentin, France
6Laboratoire de Météorologie Physique, Clermont-Ferrand, France
7TNO, Dept. Climate, Air and Sustainability, Utrecht, The Netherlands
8IPSL, Ecole Polytechnique, INSU/CNRS l'Université de Versailles, Saint-Quentin,, France
9Institut National de l'EnviRonnement industriel et des rISques, Verneuil en Halatte, France
10Institut of Chemical Engineering Sciences, Foundation for Research and Technology, Hellas, Patras, Greece
11National Center for Atmospheric Research, Boulder, USA
12AIRPARIF, Agence de Surveillance de la qualité de l'air, Paris, France
13ARIA Technologies, Boulogne-Billancourt, France

Abstract. Results of the chemistry transport model CHIMERE are compared with the measurements performed during the MEGAPOLI 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 related to the volatility of POA and the scheme of secondary organic aerosol (SOA) formation. 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 according to the air mass origin are defined. 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. All observed high concentration events are reproduced by the model mostly after long range transport, indicating that long range transport of SOA to Paris is well reproduced. 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 summer time. The advection of SOA from outside Paris is mostly responsible for the highest OA concentration levels. During advection of polluted air masses from north-east (Benelux and Central Europe), simulations indicate high levels of both anthropogenic and biogenic SOA fractions, while biogenic SOA dominates during days with advection from Southern France and Spain.

Citation: Zhang, Q. J., Beekmann, M., Drewnick, F., Freutel, F., Schneider, J., Crippa, M., Prévôt, A. S. H., Baltensperger, U., Poulain, L., Wiedensohler, A., Sciare, J., Gros, V., Borbon, A., Colomb, A., Michoud, V., Doussin, J.-F., Denier van der Gon, H. A. C., Haeffelin, M., Dupont, J.-C., Siour, G., Petetin, H., Bessagnet, B., Pandis, S. N., Hodzic, A., Sanchez, O., Honoré, C., and Perrussel, O.: Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: evaluation of the Volatility-Basis-Set approach within the CHIMERE model, Atmos. Chem. Phys. Discuss., 12, 29475-29533, doi:10.5194/acpd-12-29475-2012, 2012.
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