Atmos. Chem. Phys. Discuss., 13, 24885-24924, 2013
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Characterizing the impact of urban emissions on regional aerosol particles; airborne measurements during the MEGAPOLI experiment
E. J. Freney1, K. Sellegri1, F. Canonaco2, A. Colomb1, A. Borbon3, V. Michoud3, J.-F. Doussin3, S. Crumeyrolle4, N. Amarouch5, J.-M. Pichon1, A. S. H. Prévôt2, M. Beekmann3, and A. Schwarzenböeck1
1Laboratoire de Météorologie Physique, CNRS-Université Blaise Pascal, UMR6016, 63117, Clermont Ferrand, France
2Paul Scherrer Institute, Laboratory of Atmospheric Chemistry, 5232 Villigen PSI, Switzerland
3Laboratoire Interuniversitaire des Systemes Atmosphériques, LISA/IPSL, UMR CNRS 7583, Université Paris Est Creteil (UPEC) and Universite Paris Diderot (UPD), France
4NASA Langley Research Center, Hampton, VA 23681, USA
5CNRS, Div Tech, Inst Natl Sci Univers, UPS 855, 92195 Meudon, France

Abstract. The MEGAPOLI experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) giving detailed information of the non-refractory submicron aerosol species. The mass concentration of BC, measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), black carbon and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (−log(NOx / NOy). Plotting the equivalent ratios for the Positive Matrix Factorization (PMF) resolved species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA). Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in Mexico city, Mexico and in New England, USA. Using the measured VOCs species together with recent organic aerosol formation yields we predicted ~ 50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA, and have an impact on aerosol composition on a regional scale. They provide a quantitative measure of this impact in terms of urban plume composition and evolution relative to background aerosol composition.

Citation: Freney, E. J., Sellegri, K., Canonaco, F., Colomb, A., Borbon, A., Michoud, V., Doussin, J.-F., Crumeyrolle, S., Amarouch, N., Pichon, J.-M., Prévôt, A. S. H., Beekmann, M., and Schwarzenböeck, A.: Characterizing the impact of urban emissions on regional aerosol particles; airborne measurements during the MEGAPOLI experiment, Atmos. Chem. Phys. Discuss., 13, 24885-24924, doi:10.5194/acpd-13-24885-2013, 2013.
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