1Universités d'Aix-Marseille I, II et III – CNRS, UMR 6264: Laboratoire Chimie Provence, Equipe: IRA, 3 place Victor Hugo, 13331 Marseilles Cedex 3, France
2Laboratoire de Météorologie Physique (UMR 6016), Observatoire de Physique du Globe de Clermont-Ferrand, Université Blaise Pascal, 24 avenue des Landais, 63177 Aubière, France
Received: 22 Jan 2009 – Discussion started: 10 Mar 2009
Abstract. The fate of methacrolein in cloud evapo-condensation cycles was experimentally investigated. To this end, aqueous-phase reactions of methacrolein with OH radicals were performed (as described in Liu et al., 2009), and the obtained solutions were then nebulized and dried into a mixing chamber. ESI-MS and ESI-MS/MS analyses of the aqueous phase composition denoted the formation of high molecular weight multifunctional products containing hydroxyl, carbonyl and carboxylic acid moieties. The time profiles of these products suggest that their formation can imply radical pathways. These high molecular weight organic products are certainly responsible for the formation of secondary organic aerosol (SOA) observed during the nebulization experiments. The size, number and mass concentration of these particles increased significantly with the reaction time: after 22 h of reaction, the aerosol mass concentration was about three orders of magnitude higher than the initial aerosol quantity. The evaluated SOA yield ranged from 2 to 12%. These yields were confirmed by another estimation method based on the hygroscopic and volatility properties of the obtained SOA measured and reported by Michaud et al. (2009). These results provide, for the first time to our knowledge, strong experimental evidence that cloud processes can act, through photooxidation reactions, as important contributors to secondary organic aerosol formation in the troposphere.
Revised: 19 Jun 2009 – Accepted: 24 Jun 2009 – Published: 28 Jul 2009
El Haddad, I., Yao Liu, Nieto-Gligorovski, L., Michaud, V., Temime-Roussel, B., Quivet, E., Marchand, N., Sellegri, K., and Monod, A.: In-cloud processes of methacrolein under simulated conditions – Part 2: Formation of secondary organic aerosol, Atmos. Chem. Phys., 9, 5107-5117, doi:10.5194/acp-9-5107-2009, 2009.