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Causes and importance of new particle formation in the present-day and pre-industrial atmospheres

Gordon, Hamish and Flagan, Richard C. (2017) Causes and importance of new particle formation in the present-day and pre-industrial atmospheres. Journal of Geophysical Research. Atmospheres . ISSN 2169-897X. (In Press)

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New particle formation has been estimated to produce around half of cloud-forming particles in the present-day atmosphere, via gas-to-particle conversion. Here we assess the importance of new particle formation (NPF) for both the present-day and the pre-industrial atmospheres. We use a global aerosol model with parametrisations of NPF from previously published CLOUD chamber experiments involving sulphuric acid, ammonia, organic molecules and ions. We find that NPF produces around 67% of cloud condensation nuclei at 0.2% supersaturation (CCN0.2%) at the level of low clouds in the pre-industrial atmosphere (estimated uncertainty range 45-84%) and 54% in the present day (estimated uncertainty range 38-66%). Concerning causes, we find that the importance of biogenic volatile organic compounds (BVOCs) in NPF and CCN formation is greater than previously thought. Removing BVOCs and hence all secondary organic aerosol from our model reduces low-cloud-level CCN concentrations at 0.2% supersaturation by 26% in the present-day atmosphere and 41% in the pre-industrial. Around three-quarters of this reduction is due to the tiny fraction of the oxidation products of BVOCs that have sufficiently low volatility to be involved in NPF and early growth. Furthermore, we estimate that 40% of pre-industrial CCN0.2% are formed via ion-induced NPF, compared with 27% in the present-day, although we caution that the ion-induced fraction of NPF involving BVOCs is poorly measured at present. Our model suggests that the effect of changes in cosmic ray intensity on CCN is small and unlikely to be comparable to the effect of large variations in natural primary aerosol emissions.

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Gordon, Hamish0000-0002-1822-3224
Flagan, Richard C.0000-0001-5690-770X
Additional Information:© 2017 American Geophysical Union. Accepted manuscript online: 10 July 2017; Manuscript Accepted: 7 July 2017; Manuscript Revised: 30 June 2017; Manuscript Received: 24 March 2017. 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 coordinated 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), the FP7 EU Bacchus project under grant 603445-BACCHUS, and the Horizon 2020 projects CRESCENDO under grant agreement No 641816 and the Marie-Sklodowska-Curie project nano-CAVa No. 656994), ERC-Starting MOCAPAF grant no. 57360 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, 299574), the Finnish Funding Agency for Technology and Innovation, the Foundation, the Nessling Foundation, ERC Consolidator grant "NANODYNAMITE", No. 616075., 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, AGS1439551 and CHE1012293), the U.S. Department of Energy (grant DE-SC0014469), 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 simulation data presented in this manuscript are available from Zenodo at DOI 10.5281=zenodo.821582. The full NPF parametrisations used, and summaries of the model results, are provided as Supplementary Materials.
Funding AgencyGrant Number
Engineering and Physical Sciences Research Council (EPSRC)EP/K000225/1
Marie Curie Fellowship215072
Marie Curie Fellowship316662
European Research Council (ERC)603445-BACCHUS
European Research Council (ERC)641816
Marie Curie Fellowship656994
European Research Council (ERC)57360
European Research Council (ERC)227463
Bundesministerium für Bildung und Forschung (BMBF)01LK0902A
Bundesministerium für Bildung und Forschung (BMBF)01LK1222A
Swiss National Science Foundation200020_135307
Swiss National Science Foundation206620_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
Academy of Finland299574
Finnish Funding Agency for Technology and Innovation (Tekes)UNSPECIFIED FoundationUNSPECIFIED
Nessling FoundationUNSPECIFIED
European Research Council (ERC)616075
Fundação para a Ciência e a Tecnologia (FCT)CERN/FP/116387/2010
Swedish Research CouncilUNSPECIFIED
Russian Academy of SciencesUNSPECIFIED
Russian Foundation for Basic Research08-02-91006-CERN
Russian Foundation for Basic Research12-02-91522-CERN
Department of Energy (DOE)DE-SC0014469
Davidow FoundationUNSPECIFIED
Natural Environment Research Council (NERC)NE/J024252/1
Record Number:CaltechAUTHORS:20170710-133613695
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Official Citation:Gordon, H., Kirkby, J., Baltensperger, U., Bianchi, F., Breitenlechner, M., Curtius, J., Dias, A., Dommen, J., Donahue, N. M., Dunne, E. M., Duplissy, J., Ehrhart, S., Flagan, R. C., Frege, C., Fuchs, C., Hansel, A., Hoyle, C. R., Kulmala, M., Kürten, A., Lehtipalo, K., Makhmutov, V., Molteni, U., Rissanen, M. P., Stozkhov, Y., Tröstl, J., Tsagkogeorgas, G., Wagner, R., Williamson, C., Wimmer, D., Winkler, P. M., Yan, C. and Carslaw, K. S. (), Causes and importance of new particle formation in the present-day and pre-industrial atmospheres. J. Geophys. Res. Atmos.. Accepted Author Manuscript. doi:10.1002/2017JD026844
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:78902
Deposited By: Tony Diaz
Deposited On:10 Jul 2017 21:36
Last Modified:10 Jul 2017 21:36

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