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Global atmospheric particle formation from CERN CLOUD measurements

Dunne, Eimear M. and Gordon, Hamish and Kürten, Andreas and Almeida, João and Duplissy, Jonathan and Williamson, Christina and Ortega, Ismael K. and Pringle, Kirsty J. and Adamov, Alexey and Baltensperger, Urs and Barmet, Peter and Benduhn, Francois and Bianchi, Federico and Breitenlechner, Martin and Clarke, Antony and Curtius, Joachim and Dommen, Josef and Donahue, Neil M. and Ehrhart, Sebastian and Flagan, Richard C. and Franchin, Alessandro and Guida, Roberto and Hakala, Jani and Hansel, Armin and Heinritzi, Martin and Jokinen, Tuija and Kangasluoma, Juha and Kirkby, Jasper and Kulmala, Markku and Kupc, Agnieszka and Lawler, Michael J. and Lehtipalo, Katrianne and Makhmutov, Vladimir and Mann, Graham and Mathot, Serge and Merikanto, Joonas and Miettinen, Pasi and Nenes, Athanasios and Onnela, Antti and Rap, Alexandru and Reddington, Carly L. S. and Riccobono, Francesco and Richards, Nigel A. D. and Rissanen, Matti P. and Rondo, Linda and Sarnela, Nina and Schobesberger, Siegfried and Sengupta, Kamalika and Simon, Mario and Sipilä, Mikko and Smith, James N. and Stozkhov, Yuri and Tomé, António and Tröstl, Jasmin and Wagner, Paul E. and Wimmer, Daniela and Winkler, Paul M. and Worsnop, Douglas R. and Carslaw, Kenneth S. (2016) Global atmospheric particle formation from CERN CLOUD measurements. Science, 354 (6316). pp. 1119-1124. ISSN 0036-8075. http://resolver.caltech.edu/CaltechAUTHORS:20161107-141236938

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Abstract

Fundamental questions remain about the origin of newly formed atmospheric aerosol particles because data from laboratory measurements have been insufficient to build global models. In contrast, gas-phase chemistry models have been based on laboratory kinetics measurements for decades. Here we build a global model of aerosol formation using extensive laboratory-measured nucleation rates involving sulfuric acid, ammonia, ions and organic compounds. The simulations and a comparison with atmospheric observations show that nearly all nucleation throughout the present-day atmosphere involves ammonia or biogenic organic compounds in addition to sulfuric acid. A significant fraction of nucleation involves ions, but the relatively weak dependence on ion concentrations indicates that for the processes studied variations in cosmic ray intensity do not significantly affect climate via nucleation in the present-day atmosphere.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1126/science.aaf2649DOIArticle
http://science.sciencemag.org/content/354/6316/1119PublisherArticle
http://www.sciencemag.org/content/354/6316/1119/suppl/DC1PublisherSupplementary Material
ORCID:
AuthorORCID
Flagan, Richard C.0000-0001-5690-770X
Nenes, Athanasios0000-0003-3873-9970
Worsnop, Douglas R.0000-0002-8928-8017
Additional Information:© 2016 American Association for the Advancement of Science. 18 January 2016; accepted 12 October 2016. Published online 27 October 2016. We would like to 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, K. Ivanova, F. Josa, I. Krasin, R. Kristic, A. Laassiri, O.S. Maksumov, B. Marichy, H. Martinati, S.V. Mizin, R. Sitals, H.U. Walther, A. Wasem and M. Wilhelmsson for their important contributions to the experiment. The computer modeling simulations were performed on ARC1 and ARC2, part of the High Performance Computing facilities at the University of Leeds, UK. This work also made use of the POLARIS facility of the N8 HPC Centre of Excellence, provided and funded by the N8 consortium and EPSRC (grant no. EP/K000225/1). The Centre is co-ordinated by the Universities of Leeds and Manchester. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Networks ‘CLOUD- ITN’ (no. 215072) and ‘CLOUD-TRAIN’ (no. 316662)), ERC-Starting MOCAPAF grant no. 5736 and ERC Advanced ‘ATMNUCLE’ grant no. 227463, the German Federal Ministry of Education and Research (project nos. 01LK0902A and 01LK1222A), the Swiss National Science Foundation (project nos. 200020 135307 and 206620 141278), the Academy of Finland (Center of Excellence project no. 1118615 and other projects 135054, 133872, 251427, 139656, 139995, 137749, 141217, 141451, 138951), the Finnish Funding Agency for Technology and Innovation, the V.is.l. Foundation, the Nessling Foundation, the Austrian Science Fund (FWF; project no. J3198- N21), 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 (grants 08-02-91006-CERN and 12-02-91522-CERN), the U.S. National Science Foundation (grants AGS1136479, AGS1447056, AGC1439551 and CHE1012293), the U.S. Department of Energy (grant DE-SC0014469), the PEGASOS project funded by the European Commission under the Framework Programme 7 (FP7-ENV- 2010-265148), the Davidow Foundation, and the NERC GASSP project under grant NE/J024252/1. We acknowledge financial support from the Royal Society Wolfson Merit Award. The nucleation rates used in our manuscript are available in the supplementary materials as a CSV file.
Funders:
Funding AgencyGrant Number
CERNUNSPECIFIED
N8 ConsortiumUNSPECIFIED
Engineering and Physical Sciences Research Council (EPSRC)EP/K000225/1
Marie Curie Fellowship215072
Marie Curie Fellowship316662
European Research Council (ERC)5736
European Research Council (ERC)227463
Bundesministerium für Bildung und Forschung (BMBF)01LK0902A
Bundesministerium für Bildung und Forschung (BMBF)01LK1222A
Swiss National Science Foundation (SNSF)200020 135307
Swiss National Science Foundation (SNSF)206620 141278
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
Academy of Finland138951
Finnish Funding Agency for Technology and InnovationUNSPECIFIED
Villum FoundationUNSPECIFIED
Nessling FoundationUNSPECIFIED
FWF Der WissenschaftsfondsJ3198-N21
Fundação para a Ciência e a Tecnologia (FCT)CERN/FP/116387/2010
Swedish Research Council UNSPECIFIED
Vetenskapsrådet2011-5120
Russian Academy of SciencesUNSPECIFIED
Russian Foundation for Basic Research08-02-91006-CERN
Russian Foundation for Basic Research12-02-91522-CERN
NSFAGS1136479
NSFAGS1447056
NSFAGC1439551
NSFCHE1012293
Department of Energy (DOE)DE-SC0014469
European CommissionFP7-ENV-2010-265148
Davidow Foundation UNSPECIFIED
Natural Environment Research Council (NERC)NE/J024252/1
Royal SocietyUNSPECIFIED
Record Number:CaltechAUTHORS:20161107-141236938
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20161107-141236938
Official Citation:Global atmospheric particle formation from CERN CLOUD measurements BY EIMEAR M. DUNNE, HAMISH GORDON, ANDREAS KÜRTEN, JOÃO ALMEIDA, JONATHAN DUPLISSY, CHRISTINA WILLIAMSON, ISMAEL K. ORTEGA, KIRSTY J. PRINGLE, ALEXEY ADAMOV, URS BALTENSPERGER, PETER BARMET, FRANCOIS BENDUHN, FEDERICO BIANCHI, MARTIN BREITENLECHNER, ANTONY CLARKE, JOACHIM CURTIUS, JOSEF DOMMEN, NEIL M. DONAHUE, SEBASTIAN EHRHART, RICHARD C. FLAGAN, ALESSANDRO FRANCHIN, ROBERTO GUIDA, JANI HAKALA, ARMIN HANSEL, MARTIN HEINRITZI, TUIJA JOKINEN, JUHA KANGASLUOMA, JASPER KIRKBY, MARKKU KULMALA, AGNIESZKA KUPC, MICHAEL J. LAWLER, KATRIANNE LEHTIPALO, VLADIMIR MAKHMUTOV, GRAHAM MANN, SERGE MATHOT, JOONAS MERIKANTO, PASI MIETTINEN, ATHANASIOS NENES, ANTTI ONNELA, ALEXANDRU RAP, CARLY L. S. REDDINGTON, FRANCESCO RICCOBONO, NIGEL A. D. RICHARDS, MATTI P. RISSANEN, LINDA RONDO, NINA SARNELA, SIEGFRIED SCHOBESBERGER, KAMALIKA SENGUPTA, MARIO SIMON, MIKKO SIPILÄ, JAMES N. SMITH, YURI STOZKHOV, ANTONIO TOMÉ, JASMIN TRÖSTL, PAUL E. WAGNER, DANIELA WIMMER, PAUL M. WINKLER, DOUGLAS R. WORSNOP, KENNETH S. CARSLAW Science 02 Dec 2016: Vol. 354, Issue 6316, pp. 1119-1124 DOI: 10.1126/science.aaf2649
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:71775
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:08 Nov 2016 00:07
Last Modified:17 Nov 2017 01:01

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