Title: Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation
Authors: Kirkby, Jasper ×
Curtius, Joachim
Almeida, João
Dunne, Eimear
Duplissy, Jonathan
Ehrhart, Sebastian
Franchin, Alessandro
Gagné, Stéphanie
Ickes, Luisa
Kürten, Andreas
Kupc, Agnieszka
Metzger, Axel
Riccobono, Francesco
Rondo, Linda
Schobesberger, Siegfried
Tsagkogeorgas, Georgios
Wimmer, Daniela
Amorim, Antonio
Bianchi, Federico
Breitenlechner, Martin
David, André
Dommen, Josef
Downard, Andrew
Ehn, Mikael
Flagan, Richard C
Haider, Stefan
Hansel, Armin
Hauser, Daniel
Jud, Werner
Junninen, Heikki
Kreissl, Fabian
Kvashin, Alexander
Laaksonen, Ari
Lehtipalo, Katrianne
Lima, Jorge
Lovejoy, Edward R
Makhmutov, Vladimir
Mathot, Serge
Mikkilä, Jyri
Minginette, Pierre
Mogo, Sandra
Nieminen, Tuomo
Onnela, Antti
Pereira, Paulo
Petäjä, Tuukka
Schnitzhofer, Ralf
Seinfeld, John H
Sipilä, Mikko
Stozhkov, Yuri
Stratmann, Frank
Tomé, Antonio
Vanhanen, Joonas
Viisanen, Yrjo
Vrtala, Aron
Wagner, Paul E
Walther, Hansueli
Weingartner, Ernest
Wex, Heike
Winkler, Paul M
Carslaw, Kenneth S
Worsnop, Douglas R
Baltensperger, Urs
Kulmala, Markku #
Issue Date: Aug-2011
Publisher: Nature Publishing Group
Series Title: Nature vol:476 issue:7361 pages:429-33
Article number: 10.1038/nature10343
Abstract: Atmospheric aerosols exert an important influence on climate through their effects on stratiform cloud albedo and lifetime and the invigoration of convective storms. Model calculations suggest that almost half of the global cloud condensation nuclei in the atmospheric boundary layer may originate from the nucleation of aerosols from trace condensable vapours, although the sensitivity of the number of cloud condensation nuclei to changes of nucleation rate may be small. Despite extensive research, fundamental questions remain about the nucleation rate of sulphuric acid particles and the mechanisms responsible, including the roles of galactic cosmic rays and other chemical species such as ammonia. Here we present the first results from the CLOUD experiment at CERN. We find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume, or less, increase the nucleation rate of sulphuric acid particles more than 100-1,000-fold. Time-resolved molecular measurements reveal that nucleation proceeds by a base-stabilization mechanism involving the stepwise accretion of ammonia molecules. Ions increase the nucleation rate by an additional factor of between two and more than ten at ground-level galactic-cosmic-ray intensities, provided that the nucleation rate lies below the limiting ion-pair production rate. We find that ion-induced binary nucleation of H(2)SO(4)-H(2)O can occur in the mid-troposphere but is negligible in the boundary layer. However, even with the large enhancements in rate due to ammonia and ions, atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary-layer nucleation.
ISSN: 0028-0836
Publication status: published
KU Leuven publication type: IT
Appears in Collections:Non-KU Leuven Association publications
× corresponding author
# (joint) last author

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