Why is it so difficult to identify the onset of ice premelting?

Y Qiu, V Molinero - The journal of physical chemistry letters, 2018 - ACS Publications
The journal of physical chemistry letters, 2018ACS Publications
Premelting of ice at temperatures below 0° 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° 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 …
Premelting of ice at temperatures below 0 °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 °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.
ACS Publications
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