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Ion-induced nucleation of pure biogenic particles

Kirkby, Jasper and Craven, Jill and Flagan, Richard C. and Seinfeld, John H. and Zhang, Xuan (2016) Ion-induced nucleation of pure biogenic particles. Nature, 533 (7604). pp. 521-526. ISSN 0028-0836. http://resolver.caltech.edu/CaltechAUTHORS:20160601-132221963

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[img] Image (JPEG) (Extended Data Figure 1: Small-ion mass spectra) - Supplemental Material
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[img] Image (JPEG) (Extended Data Figure 2: HOM yields versus α-pinene oxidation rates with O3 and OH) - Supplemental Material
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[img] Image (JPEG) (Extended Data Figure 3: Proposed mechanism for the formation of the E1 and E2 surrogates via peroxy radical formation) - Supplemental Material
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[img] Image (JPEG) (Extended Data Figure 4: Typical nucleation run sequence) - Supplemental Material
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[img] Image (JPEG) (Extended Data Figure 5: Ion-induced nucleation event without H2SO4, measured in the NAIS) - Supplemental Material
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[img] Image (JPEG) (Extended Data Figure 6: Nucleation rates versus relative humidity) - Supplemental Material
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[img] Image (JPEG) (Extended Data Figure 7: Surrogate molecules chosen for quantum chemical calculations) - Supplemental Material
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[img] Image (JPEG) (Extended Data Figure 8: Relationship between cluster formation energies and equilibrium evaporation/condensation rates) - Supplemental Material
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[img] Image (JPEG) (Extended Data Table 1: Quantum chemical calculations of ELVOC cluster formation energies) - Supplemental Material
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Abstract

Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1038/nature17953DOIArticle
http://www.nature.com/nature/journal/v533/n7604/full/nature17953.htmlPublisherArticle
http://rdcu.be/iFAqPublisherFree ReadCube access
ORCID:
AuthorORCID
Flagan, Richard C.0000-0001-5690-770X
Seinfeld, John H.0000-0003-1344-4068
Additional Information:© 2016 Macmillan Publishers Limited. This work is licensed under a Creative Commons Attribution 4.0 International (CC BY 4.0) licence. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons licence, users will need to obtain permission from the licence holder to reproduce the material. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/. Received 06 July 2015; Accepted 16 March 2016; Published online 25 May 2016. We thank CERN for supporting CLOUD with important technical and financial resources, and for providing a particle beam from the CERN Proton Synchrotron. We also thank P. Carrie, L.-P. De Menezes, J. Dumollard, F. Josa, I. Krasin, R. Kristic, A. Laassiri, O. S. Maksumov, B. Marichy, H. Martinati, S. V. Mizin, R. Sitals, A. Wasem and M. Wilhelmsson for their contributions to the experiment. We thank the CSC Centre for Scientific Computing in Espoo, Finland for computer time. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network MC-ITN CLOUD-TRAIN no. 316662, EU Horizon 2020 Marie Curie grant no. 656994, ERC-Consolidator grant NANODYNAMITE no. 616075 and ERC-Advanced grant ATMNUCLE no. 227463), the German Federal Ministry of Education and Research (project no. 01LK1222A), the Swiss National Science Foundation (project nos 200020_135307, 200021_140663, 206021_144947/1 and 20FI20_149002/1), the Academy of Finland (Center of Excellence project no. 1118615), the Academy of Finland (135054, 133872, 251427, 139656, 139995, 137749, 141217, 141451), the Finnish Funding Agency for Technology and Innovation, the Väisälä Foundation, the Nessling Foundation, the Austrian Science Fund (FWF; project no. L593), the Portuguese Foundation for Science and Technology (project no. CERN/FP/116387/2010), the Swedish Research Council, Vetenskapsrådet (grant 2011-5120), the Presidium of the Russian Academy of Sciences and Russian Foundation for Basic Research (grant 12-02-91522-CERN), the UK Natural Environment Research Council (grant NE/K015966/1), the Royal Society (Wolfson Merit Award), the US National Science Foundation (grants AGS1136479, AGS1447056 and CHE1012293), Caltech ESE Grant (Davidow Foundation), Dreyfus Award EP-11-117, the French National Research Agency (ANR), the Nord-Pas de Calais, and the European Funds for Regional Economic Development (FEDER, Labex-Cappa, ANR-11-LABX-0005-01). Author Contributions: J.A., H.G., A.K., T.N., J.T. and C.W. analysed the nucleation rates; C.Fr. analysed the APi-TOF charged clusters; M.H., M.Sim. and C.Y. performed the CI-APi-TOF HOM and H2SO4 analyses; A.-K.B. analysed the PTR-TOF α-pinene; J.H.S. and X.Z. analysed the ELVOC structures and formation mechanisms; I.K.O. performed the quantum chemical calculations; A.Ad., J.A., A.Am., A.-K.B., F.B., M.B., S.B., J.Cu., J.Cr., A.D., J.Do., J.Du., S.E., C.Fr., C.Fu., H.G., M.H., C.R.H., T.J., H.J., J.Ka., J. Kim, J.Kir., M.Kr., A.K., K.L., V.M., U.M., T.N., F.P., T.P., A.P.P., M.P.R., N.S., K.S., M.Sim., M.Sip., G.S., A.T., J.T., A.W., D.W., R.W., C.W., C.Y. and P.Y. collected the data and contributed to the analysis; K.S.C., H.G., K.P., A.R., N.A.D.R., K.S. and C.E.S. evaluated the atmospheric relevance; J.Kir. wrote the manuscript; J.A., J.Do., N.M.D., C.Fr., H.G., M.H., J.H.S., M.Sim., C.W., R.W., C.Y. and X.Z. contributed to Methods and Extended Data; and U.B., K.S.C., J.Cu., J.Do., N.M.D., R.C.F., A.H., J.Kir., M.Ku., J.H.S. and D.R.W. contributed to data interpretation and editing of manuscript. All authors contributed to the development of the CLOUD facility and analysis instruments, and commented on the manuscript. The authors declare no competing financial interests.
Funders:
Funding AgencyGrant Number
CERNUNSPECIFIED
Marie Curie Fellowship316662
Marie Curie Fellowship656994
European Research Council (ERC)616075
European Research Council (ERC)227463
Bundesministerium für Bildung und Forschung (BMBF)01LK1222A
Swiss National Science Foundation (SNSF)200020_135307
Swiss National Science Foundation (SNSF)200021_140663
Swiss National Science Foundation (SNSF)206021_144947/1
Swiss National Science Foundation (SNSF)20FI20_149002/1
Academy of Finland1118615
Academy of Finland135054
Academy of Finland133872
Academy of Finland251427
Academy of Finland139656
Academy of Finland139995
Academy of Finland137749
Academy of Finland141217
Academy of Finland141451
Finnish Funding Agency for Technology and InnovationUNSPECIFIED
Väisälä FoundationUNSPECIFIED
Nessling FoundationUNSPECIFIED
FWF Der WissenschaftsfondsL593
Fundação para a Ciência e a Tecnologia (FCT)CERN/FP/116387/2010
Swedish Research CouncilUNSPECIFIED
Vetenskapsrådet2011-5120
Russian Academy of SciencesUNSPECIFIED
Russian Foundation for Basic Research12-02-91522-CERN
Natural Environment Research Council (NERC)NE/K015966/1
Royal SocietyUNSPECIFIED
NSFAGS1136479
NSFAGS1447056
NSFCHE1012293
Davidow FoundationUNSPECIFIED
Camille and Henry Dreyfus FoundationEP-11-117
Agence Nationale de la Recherche (ANR)UNSPECIFIED
Nord-Pas de CalaisUNSPECIFIED
Agence Nationale pour la Recherche (ANR)ANR-11-LABX-0005-01
European Regional Development FundUNSPECIFIED
Record Number:CaltechAUTHORS:20160601-132221963
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20160601-132221963
Official Citation:Ion-induced nucleation of pure biogenic particles Jasper Kirkby, Jonathan Duplissy, Kamalika Sengupta, Carla Frege, Hamish Gordon, Christina Williamson, Martin Heinritzi, Mario Simon, Chao Yan, João Almeida, Jasmin Tröstl, Tuomo Nieminen, Ismael K. Ortega, Robert Wagner, Alexey Adamov, Antonio Amorim, Anne-Kathrin Bernhammer, Federico Bianchi, Martin Breitenlechner, Sophia Brilke, Xuemeng Chen, Jill Craven, Antonio Dias, Sebastian Ehrhart, Richard C. Flagan, Alessandro Franchin, Claudia Fuchs, Roberto Guida, Jani Hakala, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Juha Kangasluoma, Jaeseok Kim, Manuel Krapf, Andreas Kürten, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Serge Mathot, Ugo Molteni, Antti Onnela, Otso Peräkylä, Felix Piel, Tuukka Petäjä, Arnaud P. Praplan, Kirsty Pringle, Alexandru Rap, Nigel A. D. Richards, Ilona Riipinen, Matti P. Rissanen, Linda Rondo, Nina Sarnela, Siegfried Schobesberger, Catherine E. Scott, John H. Seinfeld, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Frank Stratmann, Antonio Tomé, Annele Virtanen, Alexander L. Vogel, Andrea C. Wagner, Paul E. Wagner, Ernest Weingartner, Daniela Wimmer, Paul M. Winkler, Penglin Ye, Xuan Zhang, Armin Hansel, Josef Dommen, Neil M. Donahue, Douglas R. Worsnop, Urs Baltensperger, Markku Kulmala, Kenneth S. Carslaw & Joachim Curtius Nature 533, 521–526 (26 May 2016) doi:10.1038/nature17953
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:67550
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:01 Jun 2016 20:55
Last Modified:14 Sep 2017 22:40

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