Evolution of particle composition in CLOUD nucleation experiments

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Authors
Keskinen, Helmi
Virtanen, Annele
Joutsensaari, Jorma
Tsagkogeorgas, Georgios
Duplissy, Jonathan
Schobesberger, Siegfried
Riccobono, Francesco
Slowik, Jay Gates
Bianchi, Federico
Author (Corporation)
Publication date
2013
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01A - Journal article
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Atmospheric Chemistry and Physics
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Volume
13
Issue / Number
11
Pages / Duration
5587-5600
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Publisher / Publishing institution
Copernicus
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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.
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550 - Geowissenschaften
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1680-7324
1680-7316
Language
English
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No
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Publication status
Published
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Peer review of the complete publication
Open access category
Gold
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'https://creativecommons.org/licenses/by/4.0/'
Citation
KESKINEN, Helmi, Annele VIRTANEN, Jorma JOUTSENSAARI, Georgios TSAGKOGEORGAS, Jonathan DUPLISSY, Siegfried SCHOBESBERGER, Martin GYSEL, Francesco RICCOBONO, Jay Gates SLOWIK, Federico BIANCHI, Taina YLI-JUUTI, Katrianne LEHTIPALO, Linda RONDO, Martin BREITENLECHNER, Agnieszka KUPC, João ALMEIDA, Antonio AMORIM, Eimear M. DUNNE, Andrew J. DOWNARD, Sebastian EHRHART, Alessandro FRANCHIN, Maija K. KAJOS, Jasper KIRKBY, Andreas KÜRTEN, Tuomo NIEMINEN, Vladimir MAKHMUTOV, Serge MATHOT, Pasi MIETTINEN, Antti ONNELA, Tuukka PETÄJÄ, Arnaud PRAPLAN, Felipe D. SANTOS, Simon SCHALLHART, Mikko SIPILÄ, Yuri STOZHKOV, Antonio TOMÉ, Petri VAATTOVAARA, Daniela WIMMER, André PRÉVÔT, Josef DOMMEN, Neil M. DONAHUE, Richard C. FLAGAN, Ernest WEINGARTNER, Yrjö VIISANEN, Ilona RIIPINEN, Armin HANSEL, Joachim CURTIUS, Markku KULMALA, Douglas R. WORSNOP, Urs BALTENSPERGER, Heike WEX, Frank STRATMANN und Ari LAAKSONEN, 2013. Evolution of particle composition in CLOUD nucleation experiments. Atmospheric Chemistry and Physics. 2013. Bd. 13, Nr. 11, S. 5587–5600. DOI 10.5194/acp-13-5587-2013. Verfügbar unter: https://doi.org/10.26041/fhnw-8599