<?xml version="1.0" encoding="UTF-8"?>
<!DOCTYPE article PUBLIC "-//NLM//DTD Journal Publishing DTD v3.0 20080202//EN" "http://dtd.nlm.nih.gov/publishing/3.0/journalpublishing3.dtd">
<article xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink" article-type="research-article" dtd-version="3.0" xml:lang="en">
<front>
<journal-meta>
<journal-id journal-id-type="publisher">ACP</journal-id>
<journal-title-group>
<journal-title>Atmospheric Chemistry and Physics</journal-title>
<abbrev-journal-title abbrev-type="publisher">ACP</abbrev-journal-title>
</journal-title-group>
<issn pub-type="epub">1680-7324</issn>
<publisher><publisher-name>Copernicus GmbH</publisher-name>
<publisher-loc>Göttingen, Germany</publisher-loc>
</publisher>
</journal-meta>
<article-meta>
<article-id pub-id-type="doi">10.5194/acp-12-8589-2012</article-id>
<title-group>
<article-title>Ice cloud processing of ultra-viscous/glassy aerosol particles leads to enhanced ice nucleation ability</article-title>
</title-group>
<contrib-group><contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Wagner</surname>
<given-names>R.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Möhler</surname>
<given-names>O.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Saathoff</surname>
<given-names>H.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Schnaiter</surname>
<given-names>M.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Skrotzki</surname>
<given-names>J.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Leisner</surname>
<given-names>T.</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Wilson</surname>
<given-names>T. W.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Malkin</surname>
<given-names>T. L.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author" xlink:type="simple"><name name-style="western"><surname>Murray</surname>
<given-names>B. J.</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
</contrib-group><aff id="aff1">
<label>1</label>
<addr-line>Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research, Karlsruhe, Germany</addr-line>
</aff>
<aff id="aff2">
<label>2</label>
<addr-line>School of Earth and Environment, Woodhouse Lane, University of Leeds, Leeds LS2 9JT, UK</addr-line>
</aff>
<pub-date pub-type="epub">
<day>25</day>
<month>09</month>
<year>2012</year>
</pub-date>
<volume>12</volume>
<issue>18</issue>
<fpage>8589</fpage>
<lpage>8610</lpage>
<permissions>
<license xlink:type="simple">
<license-p>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.</license-p>
</license>
</permissions>
<self-uri xlink:href="http://www.atmos-chem-phys.net/12/8589/2012/acp-12-8589-2012.html">This article is available from http://www.atmos-chem-phys.net/12/8589/2012/acp-12-8589-2012.html</self-uri>
<self-uri xlink:href="http://www.atmos-chem-phys.net/12/8589/2012/acp-12-8589-2012.pdf">The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/8589/2012/acp-12-8589-2012.pdf</self-uri>
<abstract>
<p>The ice nucleation potential of airborne glassy aqueous aerosol particles
has been investigated by controlled expansion cooling cycles in the AIDA
aerosol and cloud chamber of the Karlsruhe Institute of Technology at
temperatures between 247 and 216 K. Four different solutes were used as
proxies for oxygenated organic matter found in the atmosphere: raffinose,
4-hydroxy-3-methoxy-DL-mandelic acid (HMMA), levoglucosan, and a
multi-component mixture of raffinose with five dicarboxylic acids and
ammonium sulphate. Similar to previous experiments with citric acid
aerosols, all particles were found to nucleate ice heterogeneously before
reaching the homogeneous freezing threshold provided that the freezing
cycles were started well below the respective glass transition temperatures
of the compounds; this is discussed in detail in a separate article. In this
contribution, we identify a further mechanism by which glassy aerosols can
promote ice nucleation below the homogeneous freezing limit. If the glassy
aerosol particles are probed in freezing cycles started only a few degrees
below their respective glass transition temperatures, they enter the liquid
regime of the state diagram upon increasing relative humidity
(moisture-induced glass-to-liquid transition) before being able to act as
heterogeneous ice nuclei. Ice formation then only occurs by homogeneous
freezing at elevated supersaturation levels. When ice forms the remaining
solution freeze concentrates and re-vitrifies. If these ice cloud processed
glassy aerosol particles are then probed in a second freezing cycle at the
same temperature, they catalyse ice formation at a supersaturation threshold
between 5 and 30% with respect to ice. By analogy with the enhanced ice
nucleation ability of insoluble ice nuclei like mineral dusts after they
nucleate ice once, we refer to this phenomenon as pre-activation. We propose
a number of possible explanations for why glassy aerosol particles that have
re-vitrified in contact with the ice crystals during the preceding
homogeneous freezing cycle exhibit pre-activation: they may retain small ice
embryos in pores, have footprints on their surface which match the ice
lattice, or simply have a much greater surface area or different surface
microstructure compared to the unprocessed glassy aerosol particles.
Pre-activation must be considered for the correct interpretation of
experimental results on the heterogeneous ice nucleation ability of glassy
aerosol particles and may provide a mechanism of producing a population of
extremely efficient ice nuclei in the upper troposphere.</p>
</abstract>
<counts><page-count count="22"/></counts>
</article-meta>
</front>
<body/>
<back>
<ref-list>
<title>References</title>
<ref id="ref1">
<label>1</label><mixed-citation publication-type="other" xlink:type="simple"> Abbatt, J. P. D., Benz, S., Cziczo, D. J., Kanji, Z., Lohmann, U., and Möhler, O.: Solid ammonium sulfate aerosols as ice nuclei: A pathway for cirrus cloud formation, Science, 313, 1770–1773, 2006. </mixed-citation>
</ref>
<ref id="ref2">
<label>2</label><mixed-citation publication-type="other" xlink:type="simple"> Bodsworth, A., Zobrist, B., and Bertram, A. K.: Inhibition of efflorescence in mixed organic-inorganic particles at temperatures less than 250 K, Phys. Chem. Chem. Phys., 12, 12259–12266, 2010. </mixed-citation>
</ref>
<ref id="ref3">
<label>3</label><mixed-citation publication-type="other" xlink:type="simple"> Debenedetti, P. G. and Stillinger, F. H.: Supercooled liquids and the glass transition, Nature, 410, 259–267, 2001. </mixed-citation>
</ref>
<ref id="ref4">
<label>4</label><mixed-citation publication-type="other" xlink:type="simple"> Higuchi, K. and Fukuta, N.: Ice in Capillaries of Solid Particles and Its Effect on Their Nucleating Ability, J. Atmos. Sci., 23, 187–190, 1966. </mixed-citation>
</ref>
<ref id="ref5">
<label>5</label><mixed-citation publication-type="other" xlink:type="simple"> Hinds, W. C., Aerosol Technology, John Wiley &amp; Sons, Inc., New York, USA, 51–55, 1999. </mixed-citation>
</ref>
<ref id="ref6">
<label>6</label><mixed-citation publication-type="other" xlink:type="simple"> Kanji, Z. A., Florea, O., and Abbatt, J. P. D.: Ice formation via deposition nucleation on mineral dust and organics: dependence of onset relative humidity on total particulate surface area, Environ. Res. Lett., 3, 025004, http://dx.doi.org/10.1088/1748-9326/3/2/025004doi:10.1088/1748-9326/3/2/025004, 2008. </mixed-citation>
</ref>
<ref id="ref7">
<label>7</label><mixed-citation publication-type="other" xlink:type="simple"> Koop, T., Luo, B. P., Tsias, A., and Peter, T.: Water activity as the determinant for homogeneous ice nucleation in aqueous solutions, Nature, 406, 611–614, 2000. </mixed-citation>
</ref>
<ref id="ref8">
<label>8</label><mixed-citation publication-type="other" xlink:type="simple"> Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere, Phys. Chem. Chem. Phys., 13, 19238–19255, 2011. </mixed-citation>
</ref>
<ref id="ref9">
<label>9</label><mixed-citation publication-type="other" xlink:type="simple"> Kovács, T., Meldrum, F. C., and Christenson, H. K.: Crystal Nucleation without Supersaturation, J. Phys. Chem. Lett., 3, 1602–1606, 2012. </mixed-citation>
</ref>
<ref id="ref10">
<label>10</label><mixed-citation publication-type="other" xlink:type="simple"> Li, K. K., Wang, F., Zeng, G., Reid, J. P., and Zhang, Y. H.: Probing the Time Scale for Bulk Equilibration and Mass Transport of Water in Amorphous Inorganic Aerosol, J. Phys. Chem. B, 115, 14397–14403, 2011. </mixed-citation>
</ref>
<ref id="ref11">
<label>11</label><mixed-citation publication-type="other" xlink:type="simple"> Malkin, T. M., Murray, B. J., Brukhno, A. V., Anwar, J., and Salzmann, C. G.: Structure of ice crystallized from supercooled water, Proc. Natl. Acad. Sci. USA, 4, 1041–1045, 2012. </mixed-citation>
</ref>
<ref id="ref12">
<label>12</label><mixed-citation publication-type="other" xlink:type="simple"> Mikhailov, E., Vlasenko, S., Martin, S. T., Koop, T., and Pöschl, U.: Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations, Atmos. Chem. Phys., 9, 9491–9522, http://dx.doi.org/10.5194/acp-9-9491-2009doi:10.5194/acp-9-9491-2009, 2009. </mixed-citation>
</ref>
<ref id="ref13">
<label>13</label><mixed-citation publication-type="other" xlink:type="simple"> Mishchenko, M. I., Travis, L. D., and Mackowski, D. W.: T-matrix computations of light scattering by nonspherical particles: A review, J. Quant. Spectrosc. Radiat. Trans., 55, 535–575, 1996. </mixed-citation>
</ref>
<ref id="ref14">
<label>14</label><mixed-citation publication-type="other" xlink:type="simple"> Möhler, O., Stetzer, O., Schaefers, S., Linke, C., Schnaiter, M., Tiede, R., Saathoff, H., Krämer, M., Mangold, A., Budz, P., Zink, P., Schreiner, J., Mauersberger, K., Haag, W., Kärcher, B., and Schurath, U.: Experimental investigation of homogeneous freezing of sulphuric acid particles in the aerosol chamber AIDA, Atmos. Chem. Phys., 3, 211–223, http://dx.doi.org/10.5194/acp-3-211-2003doi:10.5194/acp-3-211-2003, 2003. </mixed-citation>
</ref>
<ref id="ref15">
<label>15</label><mixed-citation publication-type="other" xlink:type="simple"> Möhler, O., Field, P. R., Connolly, P., Benz, S., Saathoff, H., Schnaiter, M., Wagner, R., Cotton, R., Krämer, M., Mangold, A., and Heymsfield, A. J.: Efficiency of the deposition mode ice nucleation on mineral dust particles, Atmos. Chem. Phys., 6, 3007–3021, http://dx.doi.org/10.5194/acp-6-3007-2006doi:10.5194/acp-6-3007-2006, 2006. </mixed-citation>
</ref>
<ref id="ref16">
<label>16</label><mixed-citation publication-type="other" xlink:type="simple"> Mossop, S. C.: Sublimation Nuclei, P. Phys. Soc. Lond. B, 69, 161–164, 1956. </mixed-citation>
</ref>
<ref id="ref17">
<label>17</label><mixed-citation publication-type="other" xlink:type="simple"> Murphy, D. M. and Koop, T.: Review of the vapour pressures of ice and supercooled water for atmospheric applications, Q. J. Roy. Meteorol. Soc., 131, 1539–1565, 2005. </mixed-citation>
</ref>
<ref id="ref18">
<label>18</label><mixed-citation publication-type="other" xlink:type="simple"> Murray, B. J.: Enhanced formation of cubic ice in aqueous organic acid droplets, Environ. Res. Letters, 3, 025008, http://dx.doi.org/10.1088/1748-9326/3/2/025008doi:10.1088/1748-9326/3/2/025008, 2008a. </mixed-citation>
</ref>
<ref id="ref19">
<label>19</label><mixed-citation publication-type="other" xlink:type="simple"> Murray, B. J.: Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets, Atmos. Chem. Phys., 8, 5423–5433, http://dx.doi.org/10.5194/acp-8-5423-2008doi:10.5194/acp-8-5423-2008, 2008b. </mixed-citation>
</ref>
<ref id="ref20">
<label>20</label><mixed-citation publication-type="other" xlink:type="simple"> Murray, B. J. and Bertram, A. K., Inhibition of solute crystallisation in aqueous H$^+$-NH$_4^+$-SO$_4^2-$-H&lt;sub&gt;2&lt;/sub&gt;O droplets, Phys. Chem. Chem. Phys., 10, 3287–3301, 2008. </mixed-citation>
</ref>
<ref id="ref21">
<label>21</label><mixed-citation publication-type="other" xlink:type="simple"> Murray, B. J., Wilson, T. W., Dobbie, S., Cui, Z., Al-Jumur, S. M. R. K., Möhler, O., Schnaiter, M., Wagner, R., Benz, S., Niemand, M., Saathoff, H., Ebert, V., Wagner, S., and Kärcher, B.: Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions, Nature Geosci., 3, 233–237, 2010. </mixed-citation>
</ref>
<ref id="ref22">
<label>22</label><mixed-citation publication-type="other" xlink:type="simple"> Murray, B. J., Haddrell, A. E., Peppe, S., Davies, J. F., Reid, J. P., O&apos;Sullivan, D., Price, H. C., Kumar, R., Saunders, R. W., Plane, J. M. C., Umo, N. S., and Wilson, T. W.: Glass formation and unusual hygroscopic growth of iodic acid solution droplets with relevance for iodine mediated particle formation in the marine boundary layer, Atmos. Chem. Phys., 12, 8575–8587, http://dx.doi.org/10.5194/acp-12-8575-2012doi:10.5194/acp-12-8575-2012, 2012.%blackboxwill be updated by production office </mixed-citation>
</ref>
<ref id="ref23">
<label>23</label><mixed-citation publication-type="other" xlink:type="simple"> Pruppacher, H. R. and Klett, J. D.: Microphysics of Clouds and Precipitation, Kluwer Acacdemic Publishers, Dordrecht, The Netherlands, 319–320, 337–338, 1997. </mixed-citation>
</ref>
<ref id="ref24">
<label>24</label><mixed-citation publication-type="other" xlink:type="simple"> Roberts, P. and Hallett, J.: A Laboratory Study of Ice Nucleating Properties of Some Mineral Particulates, Q. J. Roy. Meteorol. Soc., 94, 25–34, 1968. </mixed-citation>
</ref>
<ref id="ref25">
<label>25</label><mixed-citation publication-type="other" xlink:type="simple"> Schnaiter, M., Büttner, S., Möhler, O., Skrotzki, J., Vragel, M., and Wagner, R.: Influence of particle size and shape on the backscattering linear depolarisation ratio of small ice crystals – cloud chamber measurements in the context of contrail and cirrus microphysics, Atmos. Chem. Phys. Discuss., 12, 15453–15502, http://dx.doi.org/10.5194/acpd-12-15453-2012doi:10.5194/acpd-12-15453-2012, 2012. </mixed-citation>
</ref>
<ref id="ref26">
<label>26</label><mixed-citation publication-type="other" xlink:type="simple"> Shiraiwa, M., Ammann, M., Koop, T., and Pöschl, U.: Gas uptake and chemical aging of semisolid organic aerosol particles, Proc. Natl. Acad. Sci. USA, 108, 11003–11008, 2011. </mixed-citation>
</ref>
<ref id="ref27">
<label>27</label><mixed-citation publication-type="other" xlink:type="simple"> Tong, H.-J., Reid, J. P., Bones, D. L., Luo, B. P., and Krieger, U. K.: Measurements of the timescales for the mass transfer of water in glassy aerosol at low relative humidity and ambient temperature, Atmos. Chem. Phys., 11, 4739-4754, http://dx.doi.org/10.5194/acp-11-4739-2011doi:10.5194/acp-11-4739-2011, 2011. </mixed-citation>
</ref>
<ref id="ref28">
<label>28</label><mixed-citation publication-type="other" xlink:type="simple"> Vali, G.: Repeatability and randomness in heterogeneous freezing nucleation, Atmos. Chem. Phys., 8, 5017–5031, http://dx.doi.org/10.5194/acp-8-5017-2008doi:10.5194/acp-8-5017-2008, 2008. </mixed-citation>
</ref>
<ref id="ref29">
<label>29</label><mixed-citation publication-type="other" xlink:type="simple"> Wagner, R., Benz, S., Möhler, O., Saathoff, H., and Schurath, U.: Probing ice clouds by broadband mid-infrared extinction spectroscopy: case studies from ice nucleation experiments in the AIDA aerosol and cloud chamber, Atmos. Chem. Phys., 6, 4775–4800, http://dx.doi.org/10.5194/acp-6-4775-2006doi:10.5194/acp-6-4775-2006, 2006a. </mixed-citation>
</ref>
<ref id="ref30">
<label>30</label><mixed-citation publication-type="other" xlink:type="simple"> Wagner, R., Bunz, H., Linke, C., Möhler, O., Naumann, K. H., Saathoff, H., Schnaiter, M., and Schurath, U.: Chamber Simulations of Cloud Chemistry: The AIDA Chamber, in: Proceedings of the NATO Advances Research Workshop on Environmental Simulation Chambers: Application to Atmospheric Chemical Processes, held in Zakopane, Poland, from 1 to 4 October 2004, edited by: Barnes, I. and Rudzinski, K. J., Springer, 2006b. \hack </mixed-citation>
</ref>
<ref id="ref31">
<label>31</label><mixed-citation publication-type="other" xlink:type="simple"> Wagner, R., Benz, S., Bunz, H., Möhler, O., Saathoff, H., Schnaiter, M., Leisner, T., and Ebert, V.: Infrared Optical Constants of Highly Diluted Sulfuric Acid Solution Droplets at Cirrus Temperatures, J. Phys. Chem. A, 112, 11661–11676, 2008. </mixed-citation>
</ref>
<ref id="ref32">
<label>32</label><mixed-citation publication-type="other" xlink:type="simple"> Wagner, R., Linke, C., Naumann, K. H., Schnaiter, M., Vragel, M., Gangl, M., and Horvath, H.: A review of optical measurements at the aerosol and cloud chamber AIDA, J. Quant. Spectrosc. Radiat. Transfer, 110, 930–949, 2009. </mixed-citation>
</ref>
<ref id="ref33">
<label>33</label><mixed-citation publication-type="other" xlink:type="simple"> Wagner, R., Möhler, O., Saathoff, H., Schnaiter, M., and Leisner, T.: High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate, Atmos. Chem. Phys., 10, 7617–7641, http://dx.doi.org/10.5194/acp-10-7617-2010doi:10.5194/acp-10-7617-2010, 2010. </mixed-citation>
</ref>
<ref id="ref34">
<label>34</label><mixed-citation publication-type="other" xlink:type="simple"> Wagner, R., Möhler, O., Saathoff, H., Schnaiter, M., and Leisner, T.: New cloud chamber experiments on the heterogeneous ice nucleation ability of oxalic acid in the immersion mode, Atmos. Chem. Phys., 11, 2083–2110, http://dx.doi.org/10.5194/acp-11-2083-2011doi:10.5194/acp-11-2083-2011, 2011. </mixed-citation>
</ref>
<ref id="ref35">
<label>35</label><mixed-citation publication-type="other" xlink:type="simple"> Wilson, T. W., Murray, B. J., Wagner, R., Möhler, O., Saathoff, H., Schnaiter, M., Skrotzki, J., Price, H. C., Malkin, T. L., Dobbie, S., and Al-Jumur, S. M. R. K.: Glassy aerosols with a range of compositions nucleate ice heterogeneously at cirrus temperatures, Atmos. Chem. Phys., 12, 8611–8632, http://dx.doi.org/10.5194/acp-12-8611-2012doi:10.5194/acp-12-8611-2012, 2012.%blackboxwill be updated by production office </mixed-citation>
</ref>
<ref id="ref36">
<label>36</label><mixed-citation publication-type="other" xlink:type="simple"> Wise, M. E., Baustian, K. J., Koop, T., Freedman, M. A., Jensen, E. J., and Tolbert, M. A.: Depositional ice nucleation onto crystalline hydrated NaCl particles: a new mechanism for ice formation in the troposphere, Atmos. Chem. Phys., 12, 1121–1134, http://dx.doi.org/10.5194/acp-12-1121-2012doi:10.5194/acp-12-1121-2012, 2012. </mixed-citation>
</ref>
<ref id="ref37">
<label>37</label><mixed-citation publication-type="other" xlink:type="simple"> Zakharova, N. T. and Mishchenko, M. I.: Scattering properties of needlelike and platelike ice spheroids with moderate size parameters, Appl. Opt., 39, 5052–5057, 2000. </mixed-citation>
</ref>
<ref id="ref38">
<label>38</label><mixed-citation publication-type="other" xlink:type="simple"> Zobrist, B., Marcolli, C., Koop, T., Luo, B. P., Murphy, D. M., Lohmann, U., Zardini, A. A., Krieger, U. K., Corti, T., Cziczo, D. J., Fueglistaler, S., Hudson, P. K., Thomson, D. S., and Peter, T.: Oxalic acid as a heterogeneous ice nucleus in the upper troposphere and its indirect aerosol effect, Atmos. Chem. Phys., 6, 3115–3129, http://dx.doi.org/10.5194/acp-6-3115-2006doi:10.5194/acp-6-3115-2006, 2006. </mixed-citation>
</ref>
<ref id="ref39">
<label>39</label><mixed-citation publication-type="other" xlink:type="simple"> Zobrist, B., Marcolli, C., Pedernera, D. A., and Koop, T.: Do atmospheric aerosols form glasses?, Atmos. Chem. Phys., 8, 5221–5244, http://dx.doi.org/10.5194/acp-8-5221-2008doi:10.5194/acp-8-5221-2008, 2008. </mixed-citation>
</ref>
<ref id="ref40">
<label>40</label><mixed-citation publication-type="other" xlink:type="simple"> Zobrist, B., Soonsin, V., Luo, B. P., Krieger, U. K., Marcolli, C., Peter, T., and Koop, T.: Ultra-slow water diffusion in aqueous sucrose glasses, Phys. Chem. Chem. Phys., 13, 3514–3526, 2011. </mixed-citation>
</ref>
<ref id="ref41">
<label>41</label><mixed-citation publication-type="other" xlink:type="simple"> Zuberi, B., Bertram, A. K., Koop, T., Molina, L. T., and Molina, M. J.: Heterogeneous freezing of aqueous particles induced by crystallized (NH$_4)_2$SO&lt;sub&gt;4&lt;/sub&gt;, ice, and letovicite, J. Phys. Chem. A, 105, 6458–6464, 2001. </mixed-citation>
</ref>
</ref-list>
</back>
</article>