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Published March 22, 2001 | public
Journal Article

Possible mechanism of OH frequency shift dynamics in water

Abstract

The results of the recent infrared pump−probe experiment are analyzed, in which the time evolution of the spectrum of the OH-stretching vibration excited by an ultrashort laser pulse in the dilute solution HDO/D_2O was measured. To interpret the results of the experiment, a formalism developed earlier for a different application, optical transitions of the chromophoric molecules in polar solvent, is used. A mechanism of the IR shift dynamics in water is suggested, involving α-relaxation (structural relaxation), which may also be related to the dielectric behavior of water. A suggestion is made for computer simulations as well as for an experimental test of the proposed mechanism.

Additional Information

© 2001 American Chemical Society. Received: October 5, 2000; In Final Form: December 4, 2000. Publication Date (Web): February 2, 2001. We thank Prof. C. A. Angell for a very helpful discussion. It is a pleasure to acknowledge the support of the National Science Foundation and the Office of Naval Research. Y.G. acknowledges the support of the James W. Glanville Postdoctoral Scholarship in Chemistry at Caltech. It is a pleasure to dedicate this paper to Aron Kuppermann, a longtime friend and colleague, on the occasion of his 75th birthday. His insight and pioneering qualities are an inspiration not only to those who have yet to reach this age but to those of us who have.

Additional details

Created:
August 19, 2023
Modified:
October 20, 2023