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Numerical quantification of sources and phase partitioning of chemical species in cloud: application to wintertime anthropogenic air masses at the Puy de Dôme station

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Abstract

The Model of Multiphase Cloud Chemistry M2C2 has recently been extended to account for nucleation scavenging of aerosol particles in the cloud water chemical composition. This extended version has been applied to multiphase measurements available at the Puy de Dôme station for typical wintertime anthropogenic air masses. The simulated ion concentrations in cloud water are in reasonable agreement with the experimental data. The analysis of the sources of the chemical species in cloud water shows an important contribution from nucleation scavenging of particles which prevails for nitrate, sulphate and ammonium. Moreover, the simulation shows that iron, which comes only from the dissolution of aerosol particles in cloud water, has a significant contribution in the hydroxyl radical production. Finally, the simulated phase partitioning of chemical species in cloud are compared with measurements. Numerical results show an underestimation of interstitial particulate phase fraction with respect to the measurements, which could be due to an overestimation of activated mass by the model. However, the simulated number scavenging efficiency of particles agrees well with the measured value of 40% of total number of aerosol particles activated in cloud droplets. Concerning the origin of chemical species in cloud water, the model reproduces quite well the contribution of gas and aerosol scavenging estimated from measurements. In addition, the simulation provides the contribution of in-cloud chemical reactivity to cloud water concentrations.

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Acknowledgments

The authors are very grateful to Wolfram Wobrock for providing the three dimensional simulation with the Clark model. This work was supported by the “Programme National de Chimie Atmosphérique” (PNCA) of the INSU (Institut des Sciences de l’Univers) and by the ORE-BEAM (“Observatoire de Recherche en Environnement Biophysicochimie de l’Eau Atmosphérique et Modifications anthropiques”) project of the French Ministry for Research and Education. Computer resources were provided by I.D.R.I.S. (Institut du Développement et des Ressources en Informatique Scientifique, project no. 000187).

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  1. Laboratoire de Météorologie Physique, Centre National de la Recherche Scientifique, Blaise Pascal University, 24 avenue des Landais, 63177, Aubière Cedex, France

    Maud Leriche, R. Lyana Curier, Laurent Deguillaume, Dimitri Caro, Karine Sellegri & Nadine Chaumerliac

  2. Now at LA, CNRS, Paul Sabatier University, 14 avenue Edouard Belin, 31400, Toulouse, France

    Maud Leriche

  3. Now at TNO Defence Security and Safety, Electro-Optics group, P.O. Box 96864 JG, The Hague, The Netherlands

    R. Lyana Curier

  4. Now at Leibniz Institute for Tropospheric Research, Permoserstrasse 15, 04318, Leipzig, Germany

    Laurent Deguillaume

  5. Now at LSCE/IPSL, CEA/CNRS, Versailles Saint-Quentin University, Orme de Merisiers, Bat. 701, 91191, Gif-sur-Yvette Cedex, France

    Dimitri Caro

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  1. Maud Leriche
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Leriche, M., Curier, R.L., Deguillaume, L. et al. Numerical quantification of sources and phase partitioning of chemical species in cloud: application to wintertime anthropogenic air masses at the Puy de Dôme station. J Atmos Chem 57, 281–297 (2007). https://doi.org/10.1007/s10874-007-9073-y

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