Atmospheric Chemistry and Physics (Feb 2016)
Aqueous phase oxidation of sulphur dioxide by ozone in cloud droplets
- C. R. Hoyle,
- C. R. Hoyle,
- C. Fuchs,
- E. Järvinen,
- H. Saathoff,
- A. Dias,
- I. El Haddad,
- M. Gysel,
- S. C. Coburn,
- J. Tröstl,
- A.-K. Bernhammer,
- A.-K. Bernhammer,
- F. Bianchi,
- M. Breitenlechner,
- J. C. Corbin,
- J. Craven,
- J. Craven,
- N. M. Donahue,
- J. Duplissy,
- S. Ehrhart,
- C. Frege,
- H. Gordon,
- N. Höppel,
- M. Heinritzi,
- T. B. Kristensen,
- U. Molteni,
- L. Nichman,
- T. Pinterich,
- A. S. H. Prévôt,
- M. Simon,
- J. G. Slowik,
- G. Steiner,
- G. Steiner,
- G. Steiner,
- A. Tomé,
- A. L. Vogel,
- R. Volkamer,
- A. C. Wagner,
- R. Wagner,
- A. S. Wexler,
- C. Williamson,
- C. Williamson,
- C. Williamson,
- P. M. Winkler,
- C. Yan,
- A. Amorim,
- J. Dommen,
- J. Curtius,
- M. W. Gallagher,
- M. W. Gallagher,
- R. C. Flagan,
- A. Hansel,
- A. Hansel,
- J. Kirkby,
- J. Kirkby,
- M. Kulmala,
- O. Möhler,
- F. Stratmann,
- D. R. Worsnop,
- D. R. Worsnop,
- U. Baltensperger
Affiliations
- C. R. Hoyle
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- C. R. Hoyle
- WSL Institute for Snow and Avalanche Research SLF Davos, Switzerland
- C. Fuchs
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- E. Järvinen
- Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, P.O. Box 3640, 76021 Karlsruhe, Germany
- H. Saathoff
- Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, P.O. Box 3640, 76021 Karlsruhe, Germany
- A. Dias
- CERN, 1211 Geneva, Switzerland
- I. El Haddad
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- M. Gysel
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- S. C. Coburn
- Department of Chemistry and Biochemistry & CIRES, University of Colorado, Boulder, CO, USA
- J. Tröstl
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- A.-K. Bernhammer
- University of Innsbruck, Institute for Ion Physics and Applied Physics, Technikerstrasse 25, 6020 Innsbruck, Austria
- A.-K. Bernhammer
- Ionicon Analytik GmbH, Eduard-Bodem-Gasse 3, 6020 Innsbruck, Austria
- F. Bianchi
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- M. Breitenlechner
- University of Innsbruck, Institute for Ion Physics and Applied Physics, Technikerstrasse 25, 6020 Innsbruck, Austria
- J. C. Corbin
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- J. Craven
- California Institute of Technology, Department of Chemical Engineering, Pasadena, CA 91125, USA
- J. Craven
- now at: Portland Technology Development Division of Intel, Hillsboro, OR, USA
- N. M. Donahue
- Carnegie Mellon University Center for Atmospheric Particle Studies, 5000 Forbes Ave, Pittsburgh, PA 15213, USA
- J. Duplissy
- Division of Atmospheric Sciences, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
- S. Ehrhart
- CERN, 1211 Geneva, Switzerland
- C. Frege
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- H. Gordon
- CERN, 1211 Geneva, Switzerland
- N. Höppel
- Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, P.O. Box 3640, 76021 Karlsruhe, Germany
- M. Heinritzi
- Goethe University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
- T. B. Kristensen
- Leibniz Institute for Tropospheric Research, Permoserstrasse 15, 04318 Leipzig, Germany
- U. Molteni
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- L. Nichman
- School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK
- T. Pinterich
- University of Vienna, Faculty of Physics, Aerosol and Environmental Physics, Boltzmanngasse 5, 1090 Vienna, Austria
- A. S. H. Prévôt
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- M. Simon
- Goethe University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
- J. G. Slowik
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- G. Steiner
- University of Innsbruck, Institute for Ion Physics and Applied Physics, Technikerstrasse 25, 6020 Innsbruck, Austria
- G. Steiner
- Division of Atmospheric Sciences, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
- G. Steiner
- University of Vienna, Faculty of Physics, Aerosol and Environmental Physics, Boltzmanngasse 5, 1090 Vienna, Austria
- A. Tomé
- CENTRA-SIM, University of Lisbon and University of Beira Interior, 1749-016 Lisbon, Portugal
- A. L. Vogel
- CERN, 1211 Geneva, Switzerland
- R. Volkamer
- Department of Chemistry and Biochemistry & CIRES, University of Colorado, Boulder, CO, USA
- A. C. Wagner
- Goethe University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
- R. Wagner
- Division of Atmospheric Sciences, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
- A. S. Wexler
- Departments of Mechanical and Aeronautical Engineering, Civil and Environmental Engineering, and Land, Air, and Water Resources, University of California, Davis, CA, USA
- C. Williamson
- Goethe University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
- C. Williamson
- now at: Chemical Sciences Division NOAA Earth System Research Laboratory 325 Broadway R/CSD2 Boulder, CO, USA
- C. Williamson
- now at: Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO, USA
- P. M. Winkler
- University of Vienna, Faculty of Physics, Aerosol and Environmental Physics, Boltzmanngasse 5, 1090 Vienna, Austria
- C. Yan
- Division of Atmospheric Sciences, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
- A. Amorim
- CENTRA-SIM, University of Lisbon and University of Beira Interior, 1749-016 Lisbon, Portugal
- J. Dommen
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- J. Curtius
- Goethe University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
- M. W. Gallagher
- School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK
- M. W. Gallagher
- NERC Instrument PI, National Centre for Atmospheric Science (NCAS), Leeds, UK
- R. C. Flagan
- California Institute of Technology, Department of Chemical Engineering, Pasadena, CA 91125, USA
- A. Hansel
- University of Innsbruck, Institute for Ion Physics and Applied Physics, Technikerstrasse 25, 6020 Innsbruck, Austria
- A. Hansel
- Ionicon Analytik GmbH, Eduard-Bodem-Gasse 3, 6020 Innsbruck, Austria
- J. Kirkby
- CERN, 1211 Geneva, Switzerland
- J. Kirkby
- Goethe University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
- M. Kulmala
- Division of Atmospheric Sciences, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
- O. Möhler
- Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, P.O. Box 3640, 76021 Karlsruhe, Germany
- F. Stratmann
- Leibniz Institute for Tropospheric Research, Permoserstrasse 15, 04318 Leipzig, Germany
- D. R. Worsnop
- Division of Atmospheric Sciences, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
- D. R. Worsnop
- Aerodyne Research Inc., Billerica, MA 01821, USA
- U. Baltensperger
- Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
- DOI
- https://doi.org/10.5194/acp-16-1693-2016
- Journal volume & issue
-
Vol. 16
pp. 1693 – 1712
Abstract
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.
