期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 9, 期 17, 页码 5179-5182出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b02244
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资金
- National Science Foundation [CHE-1305427]
- Center for High Performance Computing at the University of Utah
Premelting of ice at temperatures below 0 degrees C is of fundamental importance for environmental processes. Various experimental techniques have been used to investigate the temperature at which liquid-like water first appears at the ice vapor interface, reporting onset temperatures from 160 to 2 degrees C. The signals that identify liquid-like order at the ice vapor interface in these studies, however, do not show a sharp initiation with temperature. That is at odds with the expected first-order nature of surface phase transitions, and consistent with recent large-scale molecular simulations that show the first premelted layer to be sparse and to develop continuously over a wide range of temperatures. Here we perform a thermodynamic analysis to elucidate the origin of the continuous formation of the first layer of liquid at the ice vapor interface. We conclude that a negative value of the line tension of the ice liquid vapor three-phase contact line is responsible for the continuous character of the transition and the sparse nature of the liquid-like domains in the incomplete first layer.
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