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Evolution of particle composition in CLOUD nucleation experiments

Keskinen, H. and Downard, A. J. and Flagan, R. C. (2013) Evolution of particle composition in CLOUD nucleation experiments. Atmospheric Chemistry and Physics, 13 (11). pp. 5587-5600. ISSN 1680-7316. http://resolver.caltech.edu/CaltechAUTHORS:20130719-102040168

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Abstract

Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD (Cosmics Leaving Outdoor Droplets) chamber experiments at CERN (Centre européen pour la recherche nucléaire). The investigation was carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovskii–Stokes–Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ~0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.5194/acp-13-5587-2013 DOIArticle
Additional Information:© 2013 Author(s). This work is distributed under the Creative Commons Attribution 3.0 License. Published by Copernicus Publications on behalf of the European Geosciences Union. Received: 22 November 2012 – Published in Atmos. Chem. Phys. Discuss.: 4 December 2012 Revised: 6 May 2013 – Accepted: 7 May 2013 – Published: 6 June 2013. 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. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network “CLOUD-ITN” grant no. 215072, the ERC-Advanced grant “ATMNUCLE” (no. 227463), the German Federal Ministry of Education and Research (project no. 01LK0902A), the Swiss National Science Foundation (project nos. 206621 125025 and 206620 130527), the Academy of Finland Centre of Excellence program (project no. 1118615), Academy of Finland (project no. 138951), the Austrian Science Fund (FWF; project nos. P19546 and L593), the Portuguese Foundation for Science and Technology (project no. CERN/FP/116387/2010), the US National Science Foundation, and the Russian Foundation for Basic Research (grant N08-02-91006-CERN).
Funders:
Funding AgencyGrant Number
EC Seventh Framework Programme215072
ERC-Advanced Grant227463
German Federal Ministry of Education and Research01LK0902A
Swiss National Science Foundation (SNSF)206621 125025
Swiss National Science Foundation (SNSF)206620 130527
Academy of Finland Centre of Excellence program1118615
Academy of Finland138951
Austrian Science Fund (FWF)P19546
Austrian Science Fund (FWF)L593
Portuguese Foundation for Science and TechnologyCERN/FP/116387/2010
NSFUNSPECIFIED
Russian Foundation for Basic ResearchN08-02-91006-CERN
Record Number:CaltechAUTHORS:20130719-102040168
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20130719-102040168
Official Citation:Keskinen, H., Virtanen, A., Joutsensaari, J., Tsagkogeorgas, G., Duplissy, J., Schobesberger, S., Gysel, M., Riccobono, F., Slowik, J. G., Bianchi, F., Yli-Juuti, T., Lehtipalo, K., Rondo, L., Breitenlechner, M., Kupc, A., Almeida, J., Amorim, A., Dunne, E. M., Downard, A. J., Ehrhart, S., Franchin, A., Kajos, M.K., Kirkby, J., Kürten, A., Nieminen, T., Makhmutov, V., Mathot, S., Miettinen, P., Onnela, A., Petäjä, T., Praplan, A., Santos, F. D., Schallhart, S., Sipilä, M., Stozhkov, Y., Tomé, A., Vaattovaara, P., Wimmer, D., Prevot, A., Dommen, J., Donahue, N. M., Flagan, R.C., Weingartner, E., Viisanen, Y., Riipinen, I., Hansel, A., Curtius, J., Kulmala, M., Worsnop, D. R., Baltensperger, U., Wex, H., Stratmann, F., and Laaksonen, A.: Evolution of particle composition in CLOUD nucleation experiments, Atmos. Chem. Phys., 13, 5587-5600, doi:10.5194/acp-13-5587-2013, 2013
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:39465
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:22 Jul 2013 22:42
Last Modified:22 Jul 2013 22:42

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