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

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Kuerten , A , Bianchi , F , Almeida , J , Kupiainen-Määttä , O , Dunne , E M , Duplissy , J , Williamson , C , Barmet , P , Breitenlechner , M , Dommen , J , Donahue , N M , Flagan , R C , Franchin , A , Gordon , H , Hakala , J , Hansel , A , Heinritzi , M , Ickes , L , Jokinen , T , Kangasluoma , J , Kim , J , Kirkby , J , Kupc , A , Lehtipalo , K , Leiminger , M , Makhmutov , V , Onnela , A , Ortega , I K , Petäjä , T , Praplan , A P , Riccobono , F , Rissanen , M P , Rondo , L , Schnitzhofer , R , Schobesberger , S , Smith , J N , Steiner , G , Stozhkov , Y , Tome , A , Trostl , J , Tsagkogeorgas , G , Wagner , P E , Wimmer , D , Ye , P , Baltensperger , U , Carslaw , K , Kulmala , M & Curtius , J 2016 , ' Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures ' , Journal of Geophysical Research : Atmospheres , vol. 121 , no. 20 , pp. 12377-12400 . https://doi.org/10.1002/2015JD023908

Title: Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures
Author: Kuerten, Andreas; Bianchi, Federico; Almeida, Joao; Kupiainen-Määttä, Oona; Dunne, Eimear M.; Duplissy, Jonathan; Williamson, Christina; Barmet, Peter; Breitenlechner, Martin; Dommen, Josef; Donahue, Neil M.; Flagan, Richard C.; Franchin, Alessandro; Gordon, Hamish; Hakala, Jani; Hansel, Armin; Heinritzi, Martin; Ickes, Luisa; Jokinen, Tuija; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Kupc, Agnieszka; Lehtipalo, Katrianne; Leiminger, Markus; Makhmutov, Vladimir; Onnela, Antti; Ortega , Ismael K.; Petäjä, Tuukka; Praplan, Arnaud P.; Riccobono, Francesco; Rissanen, Matti P.; Rondo, Linda; Schnitzhofer, Ralf; Schobesberger, Siegfried; Smith, James N.; Steiner, Gerhard; Stozhkov, Yuri; Tome, Antonio; Trostl, Jasmin; Tsagkogeorgas, Georgios; Wagner, Paul E.; Wimmer, Daniela; Ye, Penglin; Baltensperger, Urs; Carslaw, Ken; Kulmala, Markku; Curtius, Joachim
Contributor organization: Department of Physics
Polar and arctic atmospheric research (PANDA)
Date: 2016-10-27
Language: eng
Number of pages: 24
Belongs to series: Journal of Geophysical Research : Atmospheres
ISSN: 2169-897X
DOI: https://doi.org/10.1002/2015JD023908
URI: http://hdl.handle.net/10138/176238
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 298K, sulfuric acid concentrations between 5x10(5) and 1x10(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 75ion 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 248K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248K with zero added ammonia, and for higher temperatures independent of NH3 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.
Subject: nucleation
chamber study
CLOUD experiment
ion-induced nucleation
M A.S.L.
114 Physical sciences
Peer reviewed: Yes
Rights: cc_by_nc_nd
Usage restriction: openAccess
Self-archived version: publishedVersion

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