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

Kürten, Andreas and Li, Chenxi and Bianchi, Federico and Curtius, Joachim and Dias, António and Donahue, Neil M. and Duplissy, Jonathan and Flagan, Richard C. and Hakala, Jani and Jokinen, Tuija and Kirkby, Jasper and Kulmala, Markku and Laaksonen, Ari and Lehtipalo, Katrianne and Makhmutov, Vladimir and Onnela, Antti and Rissanen, Matti P. and Simon, Mario and Sipilä, Mikko and Stozhkov, Yuri and Tröstl, Jasmin and Ye, Penglin and McMurry, Peter H. (2018) New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model. Atmospheric Chemistry and Physics, 18 (2). pp. 845-863. ISSN 1680-7324. https://resolver.caltech.edu/CaltechAUTHORS:20180208-083514075

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Abstract

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 reanalyzed 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 a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (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 for the high base-to-acid ratios (∼ 100) relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1 × 10^6 and 3 × 10^7 cm^(−3), and dimethylamine mixing ratio of ∼ 40 pptv, i.e., 1 × 10^9 cm^(−3)).


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.5194/acp-18-845-2018DOIArticle
https://www.atmos-chem-phys.net/18/845/2018/PublisherArticle
ORCID:
AuthorORCID
Kürten, Andreas0000-0002-8955-4450
Bianchi, Federico0000-0003-2996-3604
Flagan, Richard C.0000-0001-5690-770X
Rissanen, Matti P.0000-0003-0463-8098
Additional Information:© Author(s) 2018. This work is distributed under the Creative Commons Attribution 4.0 License. Received: 06 Jul 2017. Discussion started: 08 Aug 2017. Revised: 24 Nov 2017. Accepted: 05 Dec 2017. Published: 23 Jan 2018. The authors declare that they have no conflict of interest. Funding from the German Federal Ministry of Education and Research (grant no. 01LK1222A) and the Marie Curie Initial Training Network “CLOUD-TRAIN” (grant no. 316662) is gratefully acknowledged. Peter H. McMurry’s and Chenxi Li’s contributions to this work were supported by the US Department of Energy’s Atmospheric System Research program and Office of Science, Office of Biological and Environmental Research, under grant number DE-SC0011780. Federico Bianchi thanks the Swiss National Science Foundation (grant no. P2EZP2_168787). Richard C. Flagan acknowledges funding from the NSF grants 1439551 and 1602086. Matti P. Rissanen appreciates funding from the Academy of Finland (project no. 299574). Katrianne Lehtipalo thanks the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement no. 656994 (nano-CAVa). Edited by: Farahnaz Khosrawi Reviewed by: three anonymous referees.
Funders:
Funding AgencyGrant Number
Bundesministerium für Bildung und Forschung (BMBF)01LK1222A
Marie Curie Fellowship316662
Department of Energy (DOE)DE-SC0011780
Swiss National Science Foundation (SNSF)P2EZP2_168787
NSFAGS-1439551
NSFAGS-1602086
Academy of Finland299574
Marie Curie Fellowship656994
Issue or Number:2
Record Number:CaltechAUTHORS:20180208-083514075
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180208-083514075
Official Citation:Kürten, A., Li, C., Bianchi, F., Curtius, J., Dias, A., Donahue, N. M., Duplissy, J., Flagan, R. C., Hakala, J., Jokinen, T., Kirkby, J., Kulmala, M., Laaksonen, A., Lehtipalo, K., Makhmutov, V., Onnela, A., Rissanen, M. P., Simon, M., Sipilä, M., Stozhkov, Y., Tröstl, J., Ye, P., and McMurry, P. H.: New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model, Atmos. Chem. Phys., 18, 845-863, https://doi.org/10.5194/acp-18-845-2018, 2018.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:84737
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:08 Feb 2018 18:34
Last Modified:09 Mar 2020 13:19

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