期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 113, 期 52, 页码 14921-14925出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1611395114
关键词
supercooled water; self-diffusion; crystallization kinetics; dynamic crossover
资金
- US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences
- Department of Energy's Office of Biological and Environmental Research
Understanding deeply supercooled water is key to unraveling many of water's anomalous properties. However, developing this understanding has proven difficult due to rapid and uncontrolled crystallization. Using a pulsed-laser-heating technique, we measure the growth rate of crystalline ice, G(T), for 180 K < T < 262 K, that is, deep within water's no man's land in ultrahigh-vacuum conditions. Isothermal measurements of G(T) are also made for 126 K <= T <= 151 K. The self-diffusion of supercooled liquid water, D(T), is obtained from G(T) using the Wilson-Frenkel model of crystal growth. For T > 237 K and P similar to 10(-8) Pa, G(T) and D(T) have super-Arrhenius (fragile) temperature dependences, but both cross over to Arrhenius (strong) behavior with a large activation energy in no man's land. The fact that G(T) and D(T) are smoothly varying rules out the hypothesis that liquid water's properties have a singularity at or near 228 K at ambient pressures. However, the results are consistent with a previous prediction for D(T) that assumed no thermodynamic transitions occur in no man's land.
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