CaltechAUTHORS
  A Caltech Library Service

Insight into Acid−Base Nucleation Experiments by Comparison of the Chemical Composition of Positive, Negative, and Neutral Clusters

Bianchi, Federico and Flagan, Richard C. (2014) Insight into Acid−Base Nucleation Experiments by Comparison of the Chemical Composition of Positive, Negative, and Neutral Clusters. Environmental Science and Technology, 48 (23). pp. 13675-13684. ISSN 0013-936X. http://resolver.caltech.edu/CaltechAUTHORS:20150108-153409377

[img] PDF (Supporting Information) - Supplemental Material
See Usage Policy.

242Kb

Use this Persistent URL to link to this item: http://resolver.caltech.edu/CaltechAUTHORS:20150108-153409377

Abstract

We investigated the nucleation of sulfuric acid together with two bases (ammonia and dimethylamine), at the CLOUD chamber at CERN. The chemical composition of positive, negative, and neutral clusters was studied using three Atmospheric Pressure interface-Time Of Flight (APi-TOF) mass spectrometers: two were operated in positive and negative mode to detect the chamber ions, while the third was equipped with a nitrate ion chemical ionization source allowing detection of neutral clusters. Taking into account the possible fragmentation that can happen during the charging of the ions or within the first stage of the mass spectrometer, the cluster formation proceeded via essentially one-to-one acid−base addition for all of the clusters, independent of the type of the base. For the positive clusters, the charge is carried by one excess protonated base, while for the negative clusters it is carried by a deprotonated acid; the same is true for the neutral clusters after these have been ionized. During the experiments involving sulfuric acid and dimethylamine, it was possible to study the appearance time for all the clusters (positive, negative, and neutral). It appeared that, after the formation of the clusters containing three molecules of sulfuric acid, the clusters grow at a similar speed, independent of their charge. The growth rate is then probably limited by the arrival rate of sulfuric acid or cluster−cluster collision.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/es502380bDOIArticle
http://pubs.acs.org/doi/abs/10.1021/es502380bPublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/es502380bPublisherSupplemental material
ORCID:
AuthorORCID
Flagan, Richard C.0000-0001-5690-770X
Additional Information:© 2014 American Chemical Society. Received: May 14, 2014; Revised: September 25, 2014; Accepted: October 7, 2014; Published: November 18, 2014. 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 and the tofTools team for support in mass spectrometry data analysis. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network “CLOUD-ITN” no. 215072, MC-ITN “CLOUD-TRAIN” no. 316662, ERC-Starting “MOCAPAF” grant no. 57360 and ERC Advanced “ATMNUCLE” grant no. 227463), theGerman 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), the Academy of Finland (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 and CHE1012293), the PEGASOS project funded by the European Commission under the Framework Programme 7 (FP7-ENV-2010-265148), and the Davidow Foundation.
Funders:
Funding AgencyGrant Number
EC Seventh Framework Programme215072
EC Seventh Framework Programme316662
ERC-Starting “MOCAPAF” grant57360
ERC Advanced “ATMNUCLE” grant227463
German Federal Ministry of Education and Research01LK0902A
German Federal Ministry of Education and Research01LK1222A
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
Finnish Funding Agency for Technology and InnovationUNSPECIFIED
V.is.l. FoundationUNSPECIFIED
Nessling FoundationUNSPECIFIED
Austrian Science FundJ3198- N21
Portuguese Foundation for Science and TechnologyCERN/FP/116387/2010
Swedish Research CouncilUNSPECIFIED
Vetenskapsrådet2011-5120
Presidium of the Russian Academy of SciencesUNSPECIFIED
Russian Foundation for Basic Research08-02-91006-CERN
Russian Foundation for Basic Research12-02-91522-CERN
NSFAGS1136479
NSFCHE1012293
European Commission under the Framework Programme 7FP7-ENV- 2010-265148
Davidow FoundationUNSPECIFIED
Record Number:CaltechAUTHORS:20150108-153409377
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20150108-153409377
Official Citation:Insight into Acid–Base Nucleation Experiments by Comparison of the Chemical Composition of Positive, Negative, and Neutral Clusters Federico Bianchi, Arnaud P. Praplan, Nina Sarnela, Josef Dommen, Andreas Kürten, Ismael K. Ortega, Siegfried Schobesberger, Heikki Junninen, Mario Simon, Jasmin Tröstl, Tuija Jokinen, Mikko Sipilä, Alexey Adamov, Antonio Amorim, Joao Almeida, Martin Breitenlechner, Jonathan Duplissy, Sebastian Ehrhart, Richard C. Flagan, Alessandro Franchin, Jani Hakala, Armin Hansel, Martin Heinritzi, Juha Kangasluoma, Helmi Keskinen, Jaeseok Kim, Jasper Kirkby, Ari Laaksonen, Michael J. Lawler, Katrianne Lehtipalo, Markus Leiminger, Vladimir Makhmutov, Serge Mathot, Antti Onnela, Tuukka Petäjä, Francesco Riccobono, Matti P. Rissanen, Linda Rondo, António Tomé, Annele Virtanen, Yrjö Viisanen, Christina Williamson, Daniela Wimmer, Paul M. Winkler, Penglin Ye, Joachim Curtius, Markku Kulmala, Douglas R. Worsnop, Neil M. Donahue, and Urs Baltensperger Environmental Science & Technology 2014 48 (23), 13675-13684
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:53403
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:13 Jan 2015 21:21
Last Modified:13 Jan 2015 21:21

Repository Staff Only: item control page