4.8 Article

Homogeneous Nucleation of Ice in Transiently-Heated, Supercooled Liquid Water Films

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JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 8, 期 23, 页码 5736-5743

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AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.7b02685

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  1. US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences
  2. Department of Energy's Office of Biological and Environmental Research

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We have investigated the nucleation and growth of crystalline ice in 0.24 mu m thick, supercooled water films adsorbed on Pt(111). The films were transiently heated with similar to 10 ns infrared laser pulses, which produced typical heating and cooling rates of similar to 10(9)-10(10) K/s. The crystallization of these water films was monitored with infrared spectroscopy. The experimental conditions were chosen to suppress ice nucleation at both the water/metal and water/vacuum interfaces. Furthermore, internal pressure increases due to curvature effects are precluded in these flat films. Therefore, the experiments were sensitive to the homogeneous ice nucleation rate from similar to 210 to 225 K. The experiments show that J(max), the maximum for the homogeneous ice nucleation rate, J(T), needs to be >= 10(26) m(-3) s(-1) and is likely to be similar to 10(29 +/- 2) m(-3) s(-1). We argue that such large nucleation rates are consistent with experiments on hyperquenched glassy water, which typically have crystalline fractions of similar to 1% or more.

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