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Volume 18, issue 2
Atmos. Chem. Phys., 18, 845-863, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Special issue: The CERN CLOUD experiment (ACP/AMT inter-journal SI)

Atmos. Chem. Phys., 18, 845-863, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 23 Jan 2018

Research article | 23 Jan 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

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 Andreas Kürten et al.
  • 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
  • 3Institute for Atmospheric and Earth System Research, University of Helsinki, 00014 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, 1211 Geneva, Switzerland
  • 8Finnish Meteorological Institute, 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 reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7nm 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 4.3nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30nm). 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 (278K, 38% relative humidity, sulfuric acid concentration between 1 × 106 and 3 × 107cm−3, and dimethylamine mixing ratio of ∼ 40pptv, i.e., 1 × 109cm−3).

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Short summary
A recent laboratory study (CLOUD) showed that new particles nucleate efficiently from sulfuric acid and dimethylamine (DMA). The reanalysis of previously published data reveals that the nucleation rates are even faster than previously assumed, i.e., nucleation can proceed at rates that are compatible with collision-controlled new particle formation for atmospheric conditions. This indicates that sulfuric acid–DMA nucleation is likely an important source of particles in the boundary layer.
A recent laboratory study (CLOUD) showed that new particles nucleate efficiently from sulfuric...