Ultrafast Hydrogen-Bond Dynamics in the Infrared Spectroscopy of Water-Reference-Cited by-同舟云学术

Ultrafast Hydrogen-Bond Dynamics in the Infrared Spectroscopy of Water

Published:2003-09-19 Issue:5640 Volume:301 Page:1698-1702
ISSN:0036-8075
Container-title:Science
language:en
Short-container-title:Science

Author:

Fecko C. J.¹²,Eaves J. D.¹²,Loparo J. J.¹²,Tokmakoff A.¹²,Geissler P. L.¹²

Affiliation:

1. Department of Chemistry, Massachusetts Institute of Technology (MIT), Cambridge, MA 02139, USA.

2. George R. Harrison Spectroscopy Laboratory, Massachusetts Institute of Technology (MIT), Cambridge, MA 02139, USA.

Abstract

We investigated rearrangements of the hydrogen-bond network in water by measuring fluctuations in the OH-stretching frequency of HOD in liquid D 2 O 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.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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