Articles | Volume 16, issue 6
Atmos. Chem. Phys., 16, 3727–3741, 2016

Special issue: Megapoli-Paris 2009/2010 campaign

Atmos. Chem. Phys., 16, 3727–3741, 2016

Research article 21 Mar 2016

Research article | 21 Mar 2016

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

Christos Fountoukis1, Athanasios G. Megaritis2, Ksakousti Skyllakou2, Panagiotis E. Charalampidis1,3, Hugo A. C. Denier van der Gon4, Monica Crippa5,6, André S. H. Prévôt6, Friederike Fachinger7, Alfred Wiedensohler8, Christodoulos Pilinis3, and Spyros N. Pandis1,2,9 Christos Fountoukis et al.
  • 1Institute of Chemical Engineering Sciences, Foundation for Research and Technology Hellas (FORTH), 26504 Patras, Greece
  • 2Department of Chemical Engineering, University of Patras, 26500 Patras, Greece
  • 3Department of Environment, University of the Aegean, 81100 Mytilene, Greece
  • 4TNO Climate, Air and Sustainability, P.O. Box 80015, 3508 TA Utrecht, the Netherlands
  • 5European Commission, Joint Research Centre (JRC), Institute for Environment and Sustainability (IES), Air and Climate Unit, Via Fermi, 2749, 21027 Ispra, Italy
  • 6Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI Villigen, Switzerland
  • 7Max Planck Institute for Chemistry, Particle Chemistry Department, Mainz, Germany
  • 8Leibniz Institute for Tropospheric Research, Leipzig, Germany
  • 9Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania, USA

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.

Short summary
We use PMCAMx with high grid resolution over Paris to simulate carbonaceous aerosol during the summer and winter MEGAPOLI campaigns. PMCAMx reproduces BC observations well. Addition of cooking organic aerosol emissions of 80 mg per day per capita is needed to reproduce the corresponding observations. While the oxygenated organic aerosol predictions during the summer are encouraging a major wintertime source appears to be missing.
Final-revised paper