Hoyle, C. R. and Craven, J. and Flagan, R. C. (2016) Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets. Atmospheric Chemistry and Physics, 16 (3). pp. 1693-1712. ISSN 1680-7324. http://resolver.caltech.edu/CaltechAUTHORS:20160325-080400747
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The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and −10 °C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion – pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that predicted using oxidation rate constants previously measured in bulk solutions. The model captured the measured aerosol growth very well for experiments performed at 10 and −10 °C, indicating that, in contrast to some previous studies, the oxidation rates of SO2 in a dispersed aqueous system can be well represented by using accepted rate constants, based on bulk measurements. To the best of our knowledge, these are the first laboratory-based measurements of aqueous phase oxidation in a dispersed, super-cooled population of droplets. The measurements are therefore important in confirming that the extrapolation of currently accepted reaction rate constants to temperatures below 0 °C is correct.
|Additional Information:||© 2016 Author(s). Published by Copernicus Publications on behalf of the European Geosciences Union. This work is distributed under the Creative Commons Attribution 3.0 License. Received: 30 October 2015. Published in Atmos. Chem. Phys. Discuss.: 1 December 2015. Revised: 28 January 2016. Accepted: 29 January 2016. Published: 12 February 2016. We thank Martin Schnaiter for his assistance with the SIMONE and PPD-2K data interpretation. The PPD-2K was made available by funding from the Deutsche Forschungsgemeinschaft under grant SCHN 1140/2-1. C. R. Hoyle was supported by the Swiss National Science Foundation (SNSF) (grant number 200021_140663). T. B. Kristensen gratefully acknowledges funding from the German Federal Ministry of Education and Research (BMBF) through the CLOUD12 project. J. Craven received funding through the Dreyfus Award EP-11-117. N. M. Donahue received funding through US National Science Foundation Grants AGS-1447056 and AGS-1439551. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network “CLOUD-TRAIN” grant no. 316662, and the German Federal Ministry of Education and Research (project no. 01LK1222A and B). Edited by: V.-M. Kerminen.|
|Official Citation:||Hoyle, C. R., Fuchs, C., Järvinen, E., Saathoff, H., Dias, A., El Haddad, I., Gysel, M., Coburn, S. C., Tröstl, J., Bernhammer, A.-K., Bianchi, F., Breitenlechner, M., Corbin, J. C., Craven, J., Donahue, N. M., Duplissy, J., Ehrhart, S., Frege, C., Gordon, H., Höppel, N., Heinritzi, M., Kristensen, T. B., Molteni, U., Nichman, L., Pinterich, T., Prévôt, A. S. H., Simon, M., Slowik, J. G., Steiner, G., Tomé, A., Vogel, A. L., Volkamer, R., Wagner, A. C., Wagner, R., Wexler, A. S., Williamson, C., Winkler, P. M., Yan, C., Amorim, A., Dommen, J., Curtius, J., Gallagher, M. W., Flagan, R. C., Hansel, A., Kirkby, J., Kulmala, M., Möhler, O., Stratmann, F., Worsnop, D. R., and Baltensperger, U.: Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets, Atmos. Chem. Phys., 16, 1693-1712, doi:10.5194/acp-16-1693-2016, 2016.|
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|Deposited By:||Ruth Sustaita|
|Deposited On:||25 Mar 2016 15:32|
|Last Modified:||25 Mar 2016 15:32|
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