ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-10-11987-2010 Comparison between simulated and observed chemical composition of fine aerosols in Paris (France) during springtime: contribution of regional versus continental emissions Sciare J. 1 d'Argouges O. 1 Zhang Q. J. 2 Sarda-Estève R. 1 Gaimoz C. 1 Gros V. 1 Beekmann M. 2 Sanchez O. 3 LSCE, Laboratoire des Sciences du Climat et de l'Environnement, unité mixte CEA-CNRS-UVSQ, UMR8212, Gif-sur-Yvette, France LISA, Laboratoire Interuniversitaire des Sciences Atmosphériques, Université Paris Est and Paris 7, CNRS, Créteil, France AIRPARIF, Agence de Surveillance de la qualité de l'air, Paris, France 16 12 2010 10 24 11987 12004 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/10/11987/2010/acp-10-11987-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/11987/2010/acp-10-11987-2010.pdf

Hourly concentrations of inorganic salts (ions) and carbonaceous material in fine aerosols (aerodynamic diameter, A.D. <2.5 μm) have been determined experimentally from fast measurements performed for a 3-week period in spring 2007 in Paris (France). The sum of these two chemical components (ions and carbonaceous aerosols) has shown to account for most of the fine aerosol mass (PM<sub>2.5</sub>). This time-resolved dataset allowed investigating the factors controlling the levels of PM<sub>2.5</sub> in Paris and showed that polluted periods with PM<sub>2.5</sub> > 15 μg m<sup>−3</sup> were characterized by air masses of continental (North-Western Europe) origin and chemical composition made by 75% of ions. By contrast, periods with clean marine air masses have shown the lowest PM<sub>2.5</sub> concentrations (typically of about 10 μg m<sup>−3</sup>); carbonaceous aerosols contributing for most of this mass (typically 75%). <br><br> In order to better discriminate between local and continental contributions to the observed chemical composition and concentrations of PM<sub>2.5</sub> over Paris, a comparative study was performed between this time-resolved dataset and the outputs of a chemistry transport model (CHIMERE), showing a relatively good capability of the model to reproduce the time-limited intense maxima observed in the field for PM<sub>2.5</sub> and ion species. Different model scenarios were then investigated switching off local and European (North-Western and Central) emissions. Results of these scenarios have clearly shown that most of the ions observed over Paris during polluted periods, were either transported or formed in-situ from gas precursors transported from Northern Europe. On the opposite, long-range transport from Europe appeared to weakly contribute to the levels of carbonaceous aerosols observed over Paris. <br><br> The model failed to properly account for the concentration levels and variability of secondary organic aerosols (SOA) determined experimentally by the EC-tracer method. The abundance of SOA (relatively to organic aerosol, OA) was as much as 75%, showing a weak dependence on air masses origin. Elevated SOA/OA ratios were also observed for air masses having residence time above ground of less than 10 h, suggesting intense emissions and/or photochemical processes leading to rapid formation of secondary organic aerosols.

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