1LSCE, Laboratoire des Sciences du Climat et de l'Environnement, unité mixte CEA-CNRS-UVSQ, UMR8212, Gif-sur-Yvette, France
2LISA, Laboratoire Interuniversitaire des Sciences Atmosphériques, Université Paris Est and Paris 7, CNRS, Créteil, France
3AIRPARIF, Agence de Surveillance de la qualité de l'air, Paris, France
Abstract. 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 (PM2.5). This time-resolved dataset allowed investigating the factors controlling the levels of PM2.5 in Paris and showed that polluted periods with PM2.5<15 μg/m3 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 PM2.5 concentrations (typically of about 10 μg/m3); carbonaceous aerosols contributing for most of this mass (typically 75%).
In order to better discriminate between regional and continental contributions to the observed chemical composition and concentrations of PM2.5 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 PM2.5 and ion species. Different model scenarios were then investigated switching off regional 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. By opposite, long-range transport from Europe appeared to poorly contribute to the levels of carbonaceous aerosols observed over Paris.
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 poor dependence on air masses origin. Elevated SOA/OA ratios were also observed for air masses having residence time above ground for less than 10 h, suggesting intense emissions and/or photochemical processes leading to rapid formation of secondary organic aerosols.