Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation

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Ehrhart , S , Ickes , L , Almeida , J , Amorim , A , Barmet , P , Bianchi , F , Dommen , J , Dunne , E M , Duplissy , J , Franchin , A , Kangasluoma , J , Kirkby , J , Kuerten , A , Kupc , A , Lehtipalo , K , Nieminen , T , Riccobono , F , Rondo , L , Schobesberger , S , Steiner , G , Tome , A , Wimmer , D , Baltensperger , U , Wagner , P E & Curtius , J 2016 , ' Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation ' , Journal of Geophysical Research : Atmospheres , vol. 121 , no. 20 , pp. 12401-12414 . https://doi.org/10.1002/2015JD023723

Title: Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation
Author: Ehrhart, Sebastian; Ickes, Luisa; Almeida, Joao; Amorim, Antonio; Barmet, Peter; Bianchi, Federico; Dommen, Josef; Dunne, Eimear M.; Duplissy, Jonathan; Franchin, Alessandro; Kangasluoma, Juha; Kirkby, Jasper; Kuerten, Andreas; Kupc, Agnieszka; Lehtipalo, Katrianne; Nieminen, Tuomo; Riccobono, Francesco; Rondo, Linda; Schobesberger, Siegfried; Steiner, Gerhard; Tome, Antonio; Wimmer, Daniela; Baltensperger, Urs; Wagner, Paul E.; Curtius, Joachim
Contributor: University of Helsinki, Paul Scherrer Institute
University of Helsinki, Helsinki Institute of Physics
University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
Date: 2016-10-27
Language: eng
Number of pages: 14
Belongs to series: Journal of Geophysical Research : Atmospheres
ISSN: 2169-897X
URI: http://hdl.handle.net/10138/176217
Abstract: Binary nucleation of sulphuric acid-water particles is expected to be an important process in the free troposphere at low temperatures. SAWNUC (Sulphuric Acid Water Nucleation) is a model of binary nucleation that is based on laboratory measurements of the binding energies of sulphuric acid and water in charged and neutral clusters. Predictions of SAWNUC are compared for the first time comprehensively with experimental binary nucleation data from the CLOUD chamber at European Organization for Nuclear Research. The experimental measurements span a temperature range of 208-292K, sulphuric acid concentrations from 110(6) to 110(9)cm(-3), and distinguish between ion-induced and neutral nucleation. Good agreement, within a factor of 5, is found between the experimental and modeled formation rates for ion-induced nucleation at 278K and below and for neutral nucleation at 208 and 223K. Differences at warm temperatures are attributed to ammonia contamination which was indicated by the presence of ammonia-sulphuric acid clusters, detected by an Atmospheric Pressure Interface Time of Flight (APi-TOF) mass spectrometer. APi-TOF measurements of the sulphuric acid ion cluster distributions (H2SO4)HSO4 with i = 0, 1, ..., 10) show qualitative agreement with the SAWNUC ion cluster distributions. Remaining differences between the measured and modeled distributions are most likely due to fragmentation in the APi-TOF. The CLOUD results are in good agreement with previously measured cluster binding energies and show the SAWNUC model to be a good representation of ion-induced and neutral binary nucleation of sulphuric acid-water clusters in the middle and upper troposphere.
Subject: ion-induced nucleation
binary nucleation
AEROSOL-PARTICLE FORMATION
ION-INDUCED NUCLEATION
ATMOSPHERIC CONDITIONS
SPHERICAL-PARTICLES
ELECTRICAL MOBILITY
MASS-SPECTROMETER
1 NM
SIZE
IONIZATION
SYSTEM
114 Physical sciences
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