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Published April 2, 2004 | public
Journal Article

Ultrafast Electron Crystallography of Interfacial Water


We report direct determination of the structures and dynamics of interfacial water on a hydrophilic surface with atomic-scale resolution using ultrafast electron crystallography. On the nanometer scale, we observed the coexistence of ordered surface water and crystallite-like ice structures, evident in the superposition of Bragg spots and Debye-Scherrer rings. The structures were determined to be dominantly cubic, but each undergoes different dynamics after the ultrafast substrate temperature jump. From changes in local bond distances (OH··O and O···O) with time, we elucidated the structural changes in the far-from-equilibrium regime at short times and near-equilibration at long times.

Additional Information

© 2004 American Association for the Advancement of Science. Received 17 December 2003; accepted 25 February 2004. Supported by the National Science Foundation. Some support was also provided by the Air Force Office of Scientific Research. F.V. acknowledges partial financial support from the Swiss National Science Foundation, and S.C. acknowledges a Millikan fellowship at Caltech. We thank N. Lewis and L. Webb for functionalizing the silicon surface.

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