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Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures

Kürten, Andreas and Flagan, Richard C. (2016) Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures. Journal of Geophysical Research. Atmospheres, 121 (20). pp. 12377-12400. ISSN 2169-897X. http://resolver.caltech.edu/CaltechAUTHORS:20170109-130950350

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Abstract

Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF rates spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 10^5 and 1 × 10^9 cm^(−3), and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximum of ~1400 parts per trillion by volume (pptv). We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm^(−3) s^(−1) to study neutral and ion-induced nucleation. We found that the contribution from ion-induced nucleation is small at temperatures between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH_3 levels. We compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1002/2015JD023908DOIArticle
http://onlinelibrary.wiley.com/doi/10.1002/2015JD023908/abstractPublisherArticle
ORCID:
AuthorORCID
Flagan, Richard C.0000-0001-5690-770X
Additional Information:© 2016 The Authors. This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made. Received 8 JUL 2015; Accepted 30 APR 2016; Published online 27 OCT 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. We thank T. Olenius for helpful discussion. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Networks “CLOUD-ITN” 215072 and “CLOUD-TRAIN” 316662, ERC-Starting “MOCAPAF” grant no. 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, 206620_130527, and 206620_141278), the Väisälä Foundation, the U.S. National Science Foundation grants (AGS1447056 and AGS1439551), the U.S. Department of Energy (contract DE-SC0014469), and the Academy of Finland via the Centre of Excellence Programme (project 1118615, grants 1133872 and 251007). The data presented in this paper are available by contacting the corresponding author A. K. (kuerten@iau.uni-frankfurt.de).
Funders:
Funding AgencyGrant Number
European Organization for Nuclear Research (CERN)UNSPECIFIED
Marie Curie Fellowship215072
Marie Curie Fellowship316662
European Research Council (ERC)57360
European Research Council (ERC)227463
Bundesministeriums für Bildung und Forschung (BMBF)01LK0902A
Bundesministeriums für Bildung und Forschung (BMBF)01LK1222A
Swiss National Science Foundation (SNSF)200020_135307
Swiss National Science Foundation (SNSF)206620_130527
Swiss National Science Foundation (SNSF)206620_141278
Väisälä FoundationUNSPECIFIED
NSFAGS-1447056
NSFAGS-1439551
Department of Energy (DOE)DE-SC0014469
Academy of Finland1118615
Academy of Finland1133872
Academy of Finland251007
Subject Keywords:nucleation; chamber study; CLOUD experiment; ion-induced nucleation
Record Number:CaltechAUTHORS:20170109-130950350
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20170109-130950350
Official Citation:Kürten, A., et al. (2016), Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures, J. Geophys. Res. Atmos., 121, 12,377–12,400, doi:10.1002/2015JD023908
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:73338
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:09 Jan 2017 21:33
Last Modified:09 Jan 2017 21:33

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