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    Insight into acid-base nucleation experiments by comparison of the chemical composition of positive, negative, and neutral clusters.
    Environ Sci Technol 2014 Dec 18;48(23):13675-84. Epub 2014 Nov 18.
    Laboratory of Atmospheric Chemistry, Paul Scherrer Institute , Villigen 5232, Switzerland.
    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.

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    Department of Chemistry and Biochemistry, University of Delaware , Newark, Delaware 19716, United States.
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    J Phys Chem A 2015 Sep 1;119(37):9670-9. Epub 2015 Sep 1.
    Division of Atmospheric Sciences, Department of Physics, University of Helsinki , P.O. Box 64, FI-00014 University of Helsinki, Finland.
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    Proc Natl Acad Sci U S A 2013 Oct 7;110(43):17223-8. Epub 2013 Oct 7.
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    Department of Chemistry and Biochemistry, University of Delaware, Newark, Delaware 19716, United States.
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