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Published December 2, 2016 | Supplemental Material + Accepted Version
Journal Article Open

Global atmospheric particle formation from CERN CLOUD measurements

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.

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.

Attached Files

Accepted Version - Global_atmospheric_particle_formation.pdf

Supplemental Material - aaf2649-Dunne-SM-data-S1.csv.zip

Supplemental Material - aaf2649-Dunne-SM.pdf

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Additional details

Created:
August 19, 2023
Modified:
October 23, 2023