Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns

Abstract. We use a three-dimensional regional chemical transport model (PMCAMx) with high grid resolution and high-resolution emissions (4 × 4 km²) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 µg m⁻³) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m⁻³) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d⁻¹ per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00–14:00 LT) and 20 % during dinner time (20:00–22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias =  −2.3 µg m⁻³) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.