New particle formation in the sulfuric acid-dimethylamine-water system : reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently, and yield particle formation rates that are compatible with boundary laye
A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently, and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are re-analyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 nm and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically-controlled) new particle formation for the conditions during the CLOUD7 experiment (278 K, 38% RH, sulfuric acid concentration between 1×106 and 3×107 cm-3 and dimethylamine mixing ratio of ~40 pptv). Finally, the simulation of atmospheric new particle formation reveals that even tiny mixing ratios of dimethylamine (0.1 pptv) yield NPF rates that could explain significant boundary layer particle formation. This highlights the need for improved speciation and quantification techniques for atmospheric gas-phase amine measurements.
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Author:Andreas Kürten, Chenxi Li, Federico Bianchi, Joachim Curtius, Antonio Dias, Neil McPherson Donahue, Jonathan Duplissy, Richard C. Flagan, Jani Hakala, Tuija Jokinen, Jasper Kirkby, Markku Kulmala, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Antti Onnela, Matti P. Rissanen, Mario Simon, Mikko Sipilä, Yuri Stozhkov, Jasmin Tröstl, Penglin Ye, Peter H. McMurry
URN:urn:nbn:de:hebis:30:3-464850
DOI:http://dx.doi.org/10.5194/acp-2017-636
ISSN:1680-7375
ISSN:1680-7367
Parent Title (English):Atmospheric chemistry and physics. Discussions
Publisher:EGU
Place of publication:Katlenburg-Lindau
Document Type:Article
Language:English
Year of Completion:2017
Date of first Publication:2017/08/08
Publishing Institution:Universitätsbibliothek Johann Christian Senckenberg
Release Date:2018/05/17
Volume:17
Pagenumber:31
First Page:1
Last Page:31
Note:
© Author(s) 2017. CC BY 4.0 License
HeBIS PPN:433881151
Institutes:Geowissenschaften
Dewey Decimal Classification:550 Geowissenschaften
Sammlungen:Universitätspublikationen
Open-Access-Publikationsfonds:Geowissenschaften / Geographie
Licence (German):License LogoCreative Commons - Namensnennung 4.0

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