ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-11-8767-2011 Heterogeneous ice nucleation: exploring the transition from stochastic to singular freezing behavior Niedermeier D. 1 Shaw R. A. 2 Hartmann S. 1 Wex H. 1 Clauss T. 1 Voigtländer J. 1 Stratmann F. 1 Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany Dept. of Physics, Michigan Technological University, Houghton, Michigan 49931, USA 30 08 2011 11 16 8767 8775 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/11/8767/2011/acp-11-8767-2011.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/8767/2011/acp-11-8767-2011.pdf

Heterogeneous ice nucleation, a primary pathway for ice formation in the atmosphere, has been described alternately as being stochastic, in direct analogy with homogeneous nucleation, or singular, with ice nuclei initiating freezing at deterministic temperatures. We present an idealized, conceptual model to explore the transition between stochastic and singular ice nucleation. This "soccer ball" model treats particles as being covered with surface sites (patches of finite area) characterized by different nucleation barriers, but with each surface site following the stochastic nature of ice embryo formation. The model provides a phenomenological explanation for seemingly contradictory experimental results obtained in our research groups. Even with ice nucleation treated fundamentally as a stochastic process this process can be masked by the heterogeneity of surface properties, as might be typical for realistic atmospheric particle populations. Full evaluation of the model findings will require experiments with well characterized ice nucleating particles and the ability to vary both temperature and waiting time for freezing.

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