Surface Crystallization of Amorphous Solid Water

(Received 1 September 2003; published 8 June 2004)We demonstrate that the crystallization of thin, supported amorphous solid water layers is initiated atthe water surface. This is concluded from the observation of sequential crystallization of amorphouswater at the surface, in the bulk, and at the water-support interface. A surface nucleation modelquantitatively reproduces the observed transformation kinetics at the three sites.