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Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison

Duplissy, J. and Flagan, R. C. (2016) Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison. Journal of Geophysical Research. Atmospheres, 121 (4). pp. 1752-1775. ISSN 2169-897X. http://resolver.caltech.edu/CaltechAUTHORS:20160427-152532390

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Abstract

We report comprehensive, demonstrably contaminant-free measurements of binary particle formation rates by sulfuric acid and water for neutral and ion-induced pathways conducted in the European Organization for Nuclear Research Cosmics Leaving Outdoor Droplets chamber. The recently developed Atmospheric Pressure interface-time of flight-mass spectrometer was used to detect contaminants in charged clusters and to identify runs free of any contaminants. Four parameters were varied to cover ambient conditions: sulfuric acid concentration (10^5 to 10^9  mol cm^(−3)), relative humidity (11% to 58%), temperature (207 K to 299 K), and total ion concentration (0 to 6800 ions cm^(−3)). Formation rates were directly measured with novel instruments at sizes close to the critical cluster size (mobility size of 1.3 nm to 3.2 nm). We compare our results with predictions from Classical Nucleation Theory normalized by Quantum Chemical calculation (QC-normalized CNT), which is described in a companion paper. The formation rates predicted by the QC-normalized CNT were extended from critical cluster sizes to measured sizes using the UHMA2 sectional particle microphysics model. Our results show, for the first time, good agreement between predicted and measured particle formation rates for the binary (neutral and ion-induced) sulfuric acid-water system. Formation rates increase with RH, sulfuric acid, and ion concentrations and decrease with temperature at fixed RH and sulfuric acid concentration. Under atmospheric conditions, neutral particle formation dominates at low temperatures, while ion-induced particle formation dominates at higher temperatures. The good agreement between the theory and our comprehensive data set gives confidence in using the QC-normalized CNT as a powerful tool to study neutral and ion-induced binary particle formation in atmospheric modeling.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1002/2015JD023539DOIArticle
http://onlinelibrary.wiley.com/doi/10.1002/2015JD023539/fullPublisherArticle
ORCID:
AuthorORCID
Flagan, R. C.0000-0001-5690-770X
Additional Information:© 2015 American Geophysical Union. Received 17 Apr 2015. Accepted 31 Aug 2015. Accepted article online 4 Sep 2015. Published online 16 Feb 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, A. Wasem, and M. Wilhelmsson for their important contributions to the experiment. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network “CLOUD-ITN” 215072, MC-ITN “CLOUD-TRAIN” 316662, ERC-Starting “MOCAPAF” grant 57360 and ERC-Advanced “ATMNUCLE” grant 227463), the German Federal Ministry of Education and Research (projects 01LK0902A and 01LK1222A), the Swiss National Science Foundation (projects 200020 135307 and 206620 141278), the Academy of Finland (Center of Excellence project 1118615), the Academy of Finland (135054, 133872, 251427, 1133872, 139656, 139995, 137749, 141217, and 141451), the Finnish Funding Agency for Technology and Innovation, the Vaisala Foundation, the Kone foundation, the Nessling Foundation, the Austrian Science Fund (FWF; project J3198-N21), the Portuguese Foundation for Science and Technology (project 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, CHE1012293, and AGS1447056), PEGASOS project (funded by the European Commission under the Framework Program 7 (FP7-ENV-2010-265148)), and the Davidow Foundation. We thank the tofTools team for providing tools for mass spectrometry analysis. In keeping with AGU's Data Policy, all process experimental data used in this paper are summarized in Table 2, and raw data used to produce the results of the paper are available from the author upon request (jonathan.duplissy@helsinki.fi).
Funders:
Funding AgencyGrant Number
CERNUNSPECIFIED
Marie Curie Fellowship215072
Marie Curie Fellowship316662
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 Foundation (SNSF)200020
Swiss National Science Foundation (SNSF)135307
Swiss National Science Foundation (SNSF)206620
Swiss National Science Foundation (SNSF)141278
Academy of Finland1118615
Academy of Finland135054
Academy of Finland133872
Academy of Finland251427
Academy of Finland1133872
Academy of Finland139656
Academy of Finland139995
Academy of Finland137749
Academy of Finland141217
Academy of Finland141451
Finnish Funding Agency for Technology and InnovationUNSPECIFIED
Vaisala FoundationUNSPECIFIED
Kone FoundationUNSPECIFIED
Nessling FoundationUNSPECIFIED
FWF Der WissenschaftsfondsJ3198-N21
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 Research08-02-91006-CERN
Russian Foundation for Basic Research12-02-91522-CERN
NSFAGS-1136479
NSFCHE-1012293
NSFAGS-1447056
European CommissionFP7-ENV-2010-265148
Davidow Foundation UNSPECIFIED
Record Number:CaltechAUTHORS:20160427-152532390
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20160427-152532390
Official Citation:Duplissy, J., et al. (2016), Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory, J. Geophys. Res. Atmos., 121, 1752–1775, doi:10.1002/2015JD023539.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:66518
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:02 May 2016 00:30
Last Modified:02 Sep 2016 19:03

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