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- Title
Ultrafast hydrogen-bond dynamics in the infrared spectroscopy of water.
- Authors
Fecko, C J; Eaves, J D; Loparo, J J; Tokmakoff, A; Geissler, P L
- Abstract
We investigated rearrangements of the hydrogen-bond network in water by measuring fluctuations in the OH-stretching frequency of HOD in liquid D2O with femtosecond infrared spectroscopy. Using simulations of an atomistic model of water, we relate these frequency fluctuations to intermolecular dynamics. The model reveals that OH frequency shifts arise from changes in the molecular electric field that acts on the proton. At short times, vibrational dephasing reflects an underdamped oscillation of the hydrogen bond with a period of 170 femtoseconds. At longer times, vibrational correlations decay on a 1.2-picosecond time scale because of collective structural reorganizations.
- Publication
Science (New York, N.Y.), 2003, Vol 301, Issue 5640, p1698
- ISSN
1095-9203
- Publication type
Journal Article
- DOI
10.1126/science.1087251