Abstract
Heterogeneous ice nucleation at the water–sapphire interface is studied using sum-frequency generation spectroscopy. We follow the response of the O–H stretch mode of interfacial water during ice nucleation as a function of time and temperature. The ice and liquid states each exhibit very distinct, largely temperature-independent responses. However, at the moment of freezing, a transient response with a significantly different intensity is observed, with a lifetime between several seconds and several minutes. The presence of this transient signal has previously been attributed to a transient phase of ice. Here, we demonstrate that the transient signal can be explained without invoking a transient ice phase, as the transient signal can simply be accounted for by a linear combination of time-dependent liquid and ice responses.
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