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      An improved approach for measuring immersion freezing in large droplets over a wide temperature range

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      a , 1 , 2
      Scientific Reports
      Nature Publishing Group

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          Abstract

          Immersion freezing (ice nucleation by particles immersed in supercooled water) is a key process for forming ice in mixed-phase clouds. Immersion freezing experiments with particles in microliter-sized (millimeter-sized) water droplets are often applied to detecting very small numbers of ice nucleating particles (INPs). However, the application of such large droplets remains confined to the detection of INPs active at temperatures much higher than the homogeneous freezing limit, because of artifacts related to freezing of water droplets without added INPs at temperatures of −25 °C or higher on a supporting substrate. Here I report a method for measuring immersion freezing in super-microliter-sized droplets over a wide temperature range. To reduce possible artifacts, droplets are pipetted onto a thin layer of Vaseline and cooled in a clean booth. In the Cryogenic Refrigerator Applied to Freezing Test (CRAFT) system, freezing of pure (Milli-Q) water droplets are limited at temperatures above −30 °C. An intercomparison of various techniques for immersion freezing experiments with reference particles (Snomax and illite NX) demonstrates that despite the use of relatively large droplets, the CRAFT setup allows for evaluating the immersion freezing activity of the particles over almost the entire temperature range (about −30 °C to 0 °C) relevant for mixed-phase cloud formation.

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          Ice nucleation by particles immersed in supercooled cloud droplets.

          The formation of ice particles in the Earth's atmosphere strongly affects the properties of clouds and their impact on climate. Despite the importance of ice formation in determining the properties of clouds, the Intergovernmental Panel on Climate Change (IPCC, 2007) was unable to assess the impact of atmospheric ice formation in their most recent report because our basic knowledge is insufficient. Part of the problem is the paucity of quantitative information on the ability of various atmospheric aerosol species to initiate ice formation. Here we review and assess the existing quantitative knowledge of ice nucleation by particles immersed within supercooled water droplets. We introduce aerosol species which have been identified in the past as potentially important ice nuclei and address their ice-nucleating ability when immersed in a supercooled droplet. We focus on mineral dusts, biological species (pollen, bacteria, fungal spores and plankton), carbonaceous combustion products and volcanic ash. In order to make a quantitative comparison we first introduce several ways of describing ice nucleation and then summarise the existing information according to the time-independent (singular) approximation. Using this approximation in combination with typical atmospheric loadings, we estimate the importance of ice nucleation by different aerosol types. According to these estimates we find that ice nucleation below about -15 °C is dominated by soot and mineral dusts. Above this temperature the only materials known to nucleate ice are biological, with quantitative data for other materials absent from the literature. We conclude with a summary of the challenges our community faces.
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            Kinetics of the homogeneous freezing of water.

            Rates of homogeneous nucleation of ice in micrometre-sized water droplets are reported. Measurements were made using a new system in which droplets were supported on a hydrophobic substrate and their phase was monitored using optical microscopy as they were cooled at a controlled rate. Our nucleation rates are in agreement, given the quoted uncertainties, with the most recent literature data. However, the level of uncertainty in the rate of homogeneous freezing remains unacceptable given the importance of homogeneous nucleation to cloud formation in the Earth's atmosphere. We go on to use the most recent thermodynamic data for cubic ice (the metastable phase thought to nucleate from supercooled water) to estimate the interfacial energy of the cubic ice-supercooled water interface. We estimate a value of 20.8 +/- 1.2 mJ m(-2) in the temperature range 234.9-236.7 K.

              Author and article information

              Journal
              Sci Rep
              Sci Rep
              Scientific Reports
              Nature Publishing Group
              2045-2322
              06 September 2016
              2016
              : 6
              : 32930
              Affiliations
              [1 ]National Institute of Polar Research , Tachikawa, Tokyo 190-8518, Japan
              [2 ]Department of Polar Science, School of Multidisciplinary Sciences, SOKENDAI (The Graduate University for Advanced Studies) , Tachikawa, Tokyo 190-8518, Japan
              Author notes
              Article
              srep32930
              10.1038/srep32930
              5011777
              27596247
              e472711d-5579-44b7-bb47-e7d5c04ce2a9
              Copyright © 2016, The Author(s)

              This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

              History
              : 08 April 2016
              : 17 August 2016
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