ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-12-8611-2012 Glassy aerosols with a range of compositions nucleate ice heterogeneously at cirrus temperatures Wilson T. W. 1 2 Murray B. J. 1 Wagner R. 3 Möhler O. 3 Saathoff H. 3 Schnaiter M. 3 Skrotzki J. 3 Price H. C. 1 Malkin T. L. 1 Dobbie S. 1 Al-Jumur S. M. R. K. 1 School of Earth and Environment, University of Leeds, UK School of Chemistry, University of Leeds, UK Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology, Germany 25 09 2012 12 18 8611 8632 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/12/8611/2012/acp-12-8611-2012.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/8611/2012/acp-12-8611-2012.pdf

Atmospheric secondary organic aerosol (SOA) is likely to exist in a semi-solid or glassy state, particularly at low temperatures and humidities. Previously, it has been shown that glassy aqueous citric acid aerosol is able to nucleate ice heterogeneously under conditions relevant to cirrus in the tropical tropopause layer (TTL). In this study we test if glassy aerosol distributions with a range of chemical compositions heterogeneously nucleate ice under cirrus conditions. Three single component aqueous solution aerosols (raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA) and levoglucosan) and one multi component aqueous solution aerosol (raffinose mixed with five dicarboxylic acids and ammonium sulphate) were studied in both the liquid and glassy states at a large cloud simulation chamber. The investigated organic compounds have similar functionality to oxidised organic material found in atmospheric aerosol and have estimated temperature/humidity induced glass transition thresholds that fall within the range predicted for atmospheric SOA. A small fraction of aerosol particles of all compositions were found to nucleate ice heterogeneously in the deposition mode at temperatures relevant to the TTL (<200 K). Raffinose and HMMA, which form glasses at higher temperatures, nucleated ice heterogeneously at temperatures as high as 214.6 and 218.5 K respectively. We present the calculated ice active surface site density, <i>n</i><sub>s</sub>, of the aerosols tested here and also of glassy citric acid aerosol as a function of relative humidity with respect to ice (RH<sub>i</sub>). We also propose a parameterisation which can be used to estimate heterogeneous ice nucleation by glassy aerosol for use in cirrus cloud models up to ~220 K. Finally, we show that heterogeneous nucleation by glassy aerosol may compete with ice nucleation on mineral dust particles in mid-latitudes cirrus.

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