Journal article

Evolution of particle composition in CLOUD nucleation experiments

Keskinen H, Virtanen A, Joutsensaari J, Tsagkogeorgas G, Duplissy J, Schobesberger S, Gysel M, Riccobono F, Slowik J, Bianchi F, Yli-Juuti T, Lehtipalo K, Rondo L, Breitenlechner M, Kupc A, Almeida J, Amorim A, Dunne E, Downard A, Ehrhart S, Franchin A, Kajos M, Kirkby J, Kürten A, Nieminen T, Makhmutov V, Mathot S, Miettinen P, Onnela A, Petäjä T, Praplan A, Santos F, Schallhart S, Sipilä M, Stozhkov Y, Tomé A, Vaattovaara P, Wimmer D, Prevot A, Dommen J, Donahue N, Flagan R, Weingartner E, Viisanen Y, Riipinen I, Hansel A, Curtius J, Kulmala M, Worsnop D, Baltensperger U, Wex H, Stratmann F, Laaksonen A ...see all

Atmospheric Chemistry and Physics, vol. 13, issue 11 (2013) pp. 5587-5600

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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 europeen pour la recherche nucleaire). 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 similar 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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