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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
© Author(s) 2017. This work is distributed under
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Research article
08 Aug 2017
Review status
This discussion paper is a preprint. A revision of this manuscript was accepted for the journal Atmospheric Chemistry and Physics (ACP) and is expected to appear here in due course.
New particle formation in the sulfuric acid-dimethy lamine-water system: Reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model
Andreas Kürten1, Chenxi Li2, Federico Bianchi3, Joachim Curtius1, António Dias4, Neil M. Donahue5, Jonathan Duplissy3, Richard C. Flagan6, Jani Hakala3, Tuija Jokinen3, Jasper Kirkby1,7, Markku Kulmala3, Ari Laaksonen8, Katrianne Lehtipalo3,9, Vladimir Makhmutov10, Antti Onnela7, Matti P. Rissanen3, Mario Simon1, Mikko Sipilä3, Yuri Stozhkov10, Jasmin Tröstl9, Penglin Ye5,11, and Peter H. McMurry2 1Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
2Department of Mechanical Engineering, University of Minnesota, 111 Church St. SE, Minneapolis, MN 55455, USA
3Department of Physics, University of Helsinki, FI-0 0014 Helsinki, Finland
4SIM, University of Lisbon, 1849-016 Lisbon, Portugal
5Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, USA
6Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, USA
7CERN, CH-1211 Geneva, Switzerland
8Finnish Meteorological Institute, FI-00101 Helsinki, Finland
9Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
10Solar and Cosmic Ray Research Laboratory, Lebedev Physical Institute, 119991 Moscow, Russia
11Aerodyne Research Inc., Billerica, Massachusetts 01821, USA
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 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.

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-dimethy lamine-water system: Reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model, Atmos. Chem. Phys. Discuss.,, in review, 2017.
Andreas Kürten et al.
Andreas Kürten et al.


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Short summary
A recent laboratory study (CLOUD chamber) showed that sulfuric acid and dimethylamine (DMA) produce aerosol particles efficiently by gas-to-particle conversion, which could be relevant for climate. This study uses an advanced method for calculating the nucleation rates and extensive process model calculations for a re-analysis of the previously published data. The results indicate that tiny DMA mixing ratios (< 1 part per trillion) can be sufficient to explain atmospheric new particle formation.
A recent laboratory study (CLOUD chamber) showed that sulfuric acid and dimethylamine (DMA)...