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Volume 18, issue 10 | Copyright

Special issue: CHemistry and AeRosols Mediterranean EXperiments (ChArMEx)...

Atmos. Chem. Phys., 18, 7287-7312, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 25 May 2018

Research article | 25 May 2018

Simulation of fine organic aerosols in the western Mediterranean area during the ChArMEx 2013 summer campaign

Arineh Cholakian1,2, Matthias Beekmann1, Augustin Colette2, Isabelle Coll1, Guillaume Siour1, Jean Sciare3,5, Nicolas Marchand4, Florian Couvidat2, Jorge Pey4,a, Valerie Gros3, Stéphane Sauvage6, Vincent Michoud6,b, Karine Sellegri7, Aurélie Colomb7, Karine Sartelet8, Helen Langley DeWitt4, Miriam Elser9,c, André S. H. Prévot9, Sonke Szidat10, and François Dulac3 Arineh Cholakian et al.
  • 1Laboratoire Inter-Universitaire des Systèmes Atmosphériques (LISA), UMR CNRS 7583, Université Paris Est Créteil et Université Paris Diderot, Institut Pierre Simon Laplace, Créteil, France
  • 2Institut National de l'Environnement Industriel et des Risques, Parc Technologique ALATA, Verneuil-en-Halatte, France
  • 3Laboratoire des Sciences du Climat et de l'Environnement, LSCE/IPSL, CEA-CNRS-UVSQ, Université Paris-Saclay, Gif-sur-Yvette, France
  • 4Aix-Marseille Université, CNRS, LCE FRE 3416, Marseille, 13331, France
  • 5The Cyprus Institute, Energy, Environment and Water Research Center, Nicosia, Cyprus
  • 6IMT Lille Douai, Univ. Lille, Département Sciences de l'Atmosphère et Génie de l'Environnement, 59000 Lille, France
  • 7LAMP, Campus universitaire des Cezeaux, 4 Avenue Blaise Pascal, 63178 Aubière, France
  • 8CEREA, Joint Laboratory École des Ponts ParisTech – EDF R and D, Université Paris-Est, 77455 Marne la Vallée, France
  • 9Paul Scherrer Institute, 5232 Villigen – PSI, Switzerland
  • 10University of Bern, Freiestrasse 3, 3012 Bern, Switzerland
  • anow at: the Spanish Geological Survey, IGME, 50006 Zaragoza, Spain
  • bnow at: Laboratoire Inter-Universitaire des Systèmes Atmosphériques (LISA), UMR CNRS 7583, Université Paris Est, France
  • cnow at: Laboratory for Advanced Analytical Technologies, Empa, Dübendorf, 8600, Switzerland

Abstract. The simulation of fine organic aerosols with CTMs (chemistry–transport models) in the western Mediterranean basin has not been studied until recently. The ChArMEx (the Chemistry-Aerosol Mediterranean Experiment) SOP 1b (Special Observation Period 1b) intensive field campaign in summer of 2013 gathered a large and comprehensive data set of observations, allowing the study of different aspects of the Mediterranean atmosphere including the formation of organic aerosols (OAs) in 3-D models. In this study, we used the CHIMERE CTM to perform simulations for the duration of the SAFMED (Secondary Aerosol Formation in the MEDiterranean) period (July to August 2013) of this campaign. In particular, we evaluated four schemes for the simulation of OA, including the CHIMERE standard scheme, the VBS (volatility basis set) standard scheme with two parameterizations including aging of biogenic secondary OA, and a modified version of the VBS scheme which includes fragmentation and formation of nonvolatile OA. The results from these four schemes are compared to observations at two stations in the western Mediterranean basin, located on Ersa, Cap Corse (Corsica, France), and at Cap Es Pinar (Mallorca, Spain). These observations include OA mass concentration, PMF (positive matrix factorization) results of different OA fractions, and 14C observations showing the fossil or nonfossil origins of carbonaceous particles. Because of the complex orography of the Ersa site, an original method for calculating an orographic representativeness error (ORE) has been developed. It is concluded that the modified VBS scheme is close to observations in all three aspects mentioned above; the standard VBS scheme without BSOA (biogenic secondary organic aerosol) aging also has a satisfactory performance in simulating the mass concentration of OA, but not for the source origin analysis comparisons. In addition, the OA sources over the western Mediterranean basin are explored. OA shows a major biogenic origin, especially at several hundred meters height from the surface; however over the Gulf of Genoa near the surface, the anthropogenic origin is of similar importance. A general assessment of other species was performed to evaluate the robustness of the simulations for this particular domain before evaluating OA simulation schemes. It is also shown that the Cap Corse site presents important orographic complexity, which makes comparison between model simulations and observations difficult. A method was designed to estimate an orographic representativeness error for species measured at Ersa and yields an uncertainty of between 50 and 85% for primary pollutants, and around 2–10% for secondary species.

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In this work, four schemes for the simulation of organic aerosols in the western Mediterranean basin are added to the CHIMERE chemistry–transport model; the resulting simulations are then compared to measurements obtained from ChArMEx. It is concluded that the scheme taking into account the fragmentation and the formation of nonvolatile organic aerosols corresponds better to measurements; the major source of this aerosol in the western Mediterranean is found to be of biogenic origin.
In this work, four schemes for the simulation of organic aerosols in the western Mediterranean...