Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation

Jasper Kirkby (), Joachim Curtius, João Almeida, Eimear Dunne, Jonathan Duplissy, Sebastian Ehrhart, Alessandro Franchin, Stéphanie Gagné, Luisa Ickes, Andreas Kürten, Agnieszka Kupc, Axel Metzger, Francesco Riccobono, Linda Rondo, Siegfried Schobesberger, Georgios Tsagkogeorgas, Daniela Wimmer, Antonio Amorim, Federico Bianchi, Martin Breitenlechner, André David, Josef Dommen, Andrew Downard, Mikael Ehn, Richard C. Flagan, Stefan Haider, Armin Hansel, Daniel Hauser, Werner Jud, Heikki Junninen, Fabian Kreissl, Alexander Kvashin, Ari Laaksonen, Katrianne Lehtipalo, Jorge Lima, Edward R. Lovejoy, Vladimir Makhmutov, Serge Mathot, Jyri Mikkilä, Pierre Minginette, Sandra Mogo, Tuomo Nieminen, Antti Onnela, Paulo Pereira, Tuukka Petäjä, Ralf Schnitzhofer, John H. Seinfeld, Mikko Sipilä, Yuri Stozhkov, Frank Stratmann, Antonio Tomé, Joonas Vanhanen, Yrjo Viisanen, Aron Vrtala, Paul E. Wagner, Hansueli Walther, Ernest Weingartner, Heike Wex, Paul M. Winkler, Kenneth S. Carslaw, Douglas R. Worsnop, Urs Baltensperger and Markku Kulmala
Additional contact information
Jasper Kirkby: CERN
Joachim Curtius: Goethe-University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
João Almeida: Goethe-University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
Eimear Dunne: University of Leeds, School of Earth and Environment, LS2-9JT Leeds, United Kingdom
Jonathan Duplissy: CERN
Sebastian Ehrhart: Goethe-University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
Alessandro Franchin: University of Helsinki, FI-00014 Helsinki, Finland
Stéphanie Gagné: University of Helsinki, FI-00014 Helsinki, Finland
Luisa Ickes: Goethe-University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
Andreas Kürten: Goethe-University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
Agnieszka Kupc: University of Vienna, Faculty of Physics, 1090 Vienna, Austria
Axel Metzger: Ionicon Analytik GmbH and University of Innsbruck, Institute for Ion and Applied Physics, 6020 Innsbruck, Austria
Francesco Riccobono: Paul Scherrer Institut, Laboratory of Atmospheric Chemistry, CH-5232 Villigen, Switzerland
Linda Rondo: Goethe-University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
Siegfried Schobesberger: University of Helsinki, FI-00014 Helsinki, Finland
Georgios Tsagkogeorgas: Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany
Daniela Wimmer: Goethe-University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
Antonio Amorim: SIM, University of Lisbon and University of Beira Interior, 1749-016 Lisbon, Portugal
Federico Bianchi: Paul Scherrer Institut, Laboratory of Atmospheric Chemistry, CH-5232 Villigen, Switzerland
Martin Breitenlechner: Ionicon Analytik GmbH and University of Innsbruck, Institute for Ion and Applied Physics, 6020 Innsbruck, Austria
André David: CERN
Josef Dommen: Paul Scherrer Institut, Laboratory of Atmospheric Chemistry, CH-5232 Villigen, Switzerland
Andrew Downard: California Institute of Technology, Pasadena, California 91125, USA
Mikael Ehn: University of Helsinki, FI-00014 Helsinki, Finland
Richard C. Flagan: California Institute of Technology, Pasadena, California 91125, USA
Stefan Haider: CERN
Armin Hansel: Ionicon Analytik GmbH and University of Innsbruck, Institute for Ion and Applied Physics, 6020 Innsbruck, Austria
Daniel Hauser: Ionicon Analytik GmbH and University of Innsbruck, Institute for Ion and Applied Physics, 6020 Innsbruck, Austria
Werner Jud: Ionicon Analytik GmbH and University of Innsbruck, Institute for Ion and Applied Physics, 6020 Innsbruck, Austria
Heikki Junninen: University of Helsinki, FI-00014 Helsinki, Finland
Fabian Kreissl: Goethe-University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany
Alexander Kvashin: Lebedev Physical Institute, Solar and Cosmic Ray Research Laboratory, 119991 Moscow, Russia
Ari Laaksonen: University of Eastern Finland, FI-70211 Kuopio, Finland
Katrianne Lehtipalo: University of Helsinki, FI-00014 Helsinki, Finland
Jorge Lima: SIM, University of Lisbon and University of Beira Interior, 1749-016 Lisbon, Portugal
Edward R. Lovejoy: NOAA Earth System Research Laboratory
Vladimir Makhmutov: Lebedev Physical Institute, Solar and Cosmic Ray Research Laboratory, 119991 Moscow, Russia
Serge Mathot: CERN
Jyri Mikkilä: University of Helsinki, FI-00014 Helsinki, Finland
Pierre Minginette: CERN
Sandra Mogo: SIM, University of Lisbon and University of Beira Interior, 1749-016 Lisbon, Portugal
Tuomo Nieminen: University of Helsinki, FI-00014 Helsinki, Finland
Antti Onnela: CERN
Paulo Pereira: SIM, University of Lisbon and University of Beira Interior, 1749-016 Lisbon, Portugal
Tuukka Petäjä: University of Helsinki, FI-00014 Helsinki, Finland
Ralf Schnitzhofer: Ionicon Analytik GmbH and University of Innsbruck, Institute for Ion and Applied Physics, 6020 Innsbruck, Austria
John H. Seinfeld: California Institute of Technology, Pasadena, California 91125, USA
Mikko Sipilä: University of Helsinki, FI-00014 Helsinki, Finland
Yuri Stozhkov: Lebedev Physical Institute, Solar and Cosmic Ray Research Laboratory, 119991 Moscow, Russia
Frank Stratmann: Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany
Antonio Tomé: SIM, University of Lisbon and University of Beira Interior, 1749-016 Lisbon, Portugal
Joonas Vanhanen: University of Helsinki, FI-00014 Helsinki, Finland
Yrjo Viisanen: Finnish Meteorological Institute, FI-00101 Helsinki, Finland
Aron Vrtala: University of Vienna, Faculty of Physics, 1090 Vienna, Austria
Paul E. Wagner: University of Vienna, Faculty of Physics, 1090 Vienna, Austria
Hansueli Walther: Paul Scherrer Institut, Laboratory of Atmospheric Chemistry, CH-5232 Villigen, Switzerland
Ernest Weingartner: Paul Scherrer Institut, Laboratory of Atmospheric Chemistry, CH-5232 Villigen, Switzerland
Heike Wex: Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany
Paul M. Winkler: University of Vienna, Faculty of Physics, 1090 Vienna, Austria
Kenneth S. Carslaw: University of Leeds, School of Earth and Environment, LS2-9JT Leeds, United Kingdom
Douglas R. Worsnop: University of Helsinki, FI-00014 Helsinki, Finland
Urs Baltensperger: Paul Scherrer Institut, Laboratory of Atmospheric Chemistry, CH-5232 Villigen, Switzerland
Markku Kulmala: University of Helsinki, FI-00014 Helsinki, Finland

Nature, 2011, vol. 476, issue 7361, 429-433

Abstract: Cloud cover at CERN A substantial source of cloud condensation nuclei in the atmospheric boundary layer is thought to originate from the nucleation of trace sulphuric acid vapour. Despite extensive research, we still lack a quantitative understanding of the nucleation mechanism and the possible role of cosmic rays, creating one of the largest uncertainties in atmospheric models and climate predictions. Jasper Kirkby and colleagues present the first results from the CLOUD experiment at CERN, which studies nucleation and other ion-aerosol cloud interactions under precisely controlled conditions. They find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume increase the nucleation rate of sulphuric acid particles by more than a factor of 100 to 1,000. They also find that ion-induced binary nucleation of H2SO4–H2O can occur in the mid-troposphere, but is negligible in the boundary layer and so additional species are necessary. Even with the large enhancements in rate caused by ammonia and ions, they conclude that atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary layer nucleation.

Date: 2011
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DOI: 10.1038/nature10343

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