Evolution of particle composition in CLOUD nucleation experiments

  • 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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Author:Helmi Keskinen, Annele Virtanen, Jorma Joutsensaari, Georgios Tsagkogeorgas, Jonathan DuplissyORCiD, Siegfried SchobesbergerORCiDGND, Martin Gysel, Francesco Riccobono, Jay G. Slowik, Federico BianchiORCiDGND, Taina Yli-Juuti, Katrianne LehtipaloORCiDGND, Linda Rondo, Martin BreitenlechnerORCiD, Agnieszka Kupc, Joao Almeida, António Amorin, Eimear M. Dunne, Andrew J. Downward, Sebastian Ehrhart, Alessandro Franchin, Maija K. Kajos, Jasper KirkbyORCiD, Christoph Andreas KürtenORCiDGND, Tuomo Nieminen, Vladimir MakhmutovORCiD, Serge Mathot, Pasi Miettinen, Antti OnnelaORCiD, Tuukka Petäjä, Arnaud Patrick Praplan, Filipe Duarte Santos, Simon Schallhart, Mikko SipiläORCiD, Yuri Stozhkov, Antonio Tomé, Petri Vaattovaara, Daniela WimmerORCiDGND, André Stephan Henry Prévôt, Josef Dommen, Neil McPherson DonahueORCiDGND, Richard C. FlaganORCiD, Ernest Weingartner, Yrjö Viisanen, Ilona RiipinenORCiD, Armin HanselORCiD, Joachim CurtiusORCiD, Markku KulmalaORCiDGND, Douglas R. WorsnopORCiD, Urs BaltenspergerORCiDGND, Heike WexORCiDGND, Frank StratmannORCiDGND, Ari Laaksonen
Parent Title (English):Atmospheric chemistry and physics
Place of publication:Katlenburg-Lindau.
Document Type:Article
Date of Publication (online):2013/06/06
Date of first Publication:2013/06/06
Publishing Institution:Universitätsbibliothek Johann Christian Senckenberg
Release Date:2013/10/09
Page Number:14
First Page:5587
Last Page:5600
© Author(s) 2013. This work is distributed under the Creative Commons Attribution 3.0 License.
Institutes:Geowissenschaften / Geographie / Geowissenschaften
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 55 Geowissenschaften, Geologie / 550 Geowissenschaften
Licence (German):License LogoCreative Commons - Namensnennung 3.0