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Physical Review Letters

Ultrafast Vibrational Dephasing of Liquid Water

Jens Stenger, Dorte Madsen, Peter M. Hamm, Erik T. J. Nibbering, Thomas Elsaesser

Published Jun 20, 2001• 231 citations
Publisher

Abstract

We present the first infrared photon echo study of liquid water. For the O-H stretch vibration of HDO in ${\mathrm{D}}_{2}\mathrm{O}$, femtosecond four-wave mixing experiments reveal an extraordinary short pure dephasing time ${T}_{2}^{*}$ on the order of 90 fs. This unusually fast time scale of dephasing is rationalized by taking into account the large anharmonicity of the hydrogen bonded O-H stretching mode.

DOI
10.1103/physrevlett.87.027401

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We present the first infrared photon echo study of liquid water. For the O-H stretch vibration of HDO in D2O{\mathrm{D}}_{2}\mathrm{O}D2​O, femtosecond four-wave mixing experiments reveal an extraordinary short pure dephasing time T2∗{T}_{2}^{*}T2∗​ on the order of 90 fs. This unusually fast time scale of dephasing is rationalized by taking into account the large anharmonicity of the hydrogen bonded O-H stretching mode.
The first infrared vibrational photon echo experiments conducted in a liquid and a glass are reported. The experiments were performed on the CO stretching mode of tungsten hexacarbonyl at 5.1 \ensuremath{\mu}m (1960 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) in 2-methyltetrahydrofuran over the temperature range 300 to 16 K using picosecond pulses from the free electron laser at Stanford University. In addition, the first vibrational population relaxation measurements spanning a temperature range that takes a system from a liquid to a supercooled liquid to a glass are reported.
Heterodyne-detected transient grating experiments on the OH-stretch mode of HDO dissolved in D2O{\mathrm{D}}_{2}\mathrm{O}D2​O resolve two distinctly different contributions originating from the initially excited OH stretch and the OD stretch which is thermally activated during the OH population relaxation. It is demonstrated that interference of both contributions greatly affects the outcome of IR photon echo experiments.
The first infrared vibrational photon echo experiments conducted in a liquid and a glass are reported. The experiments were performed on the CO stretching mode of tungsten hexacarbonyl at 5.1 micrometers (1960 cm-1) in 2-methyltetrahydrofuran over the temperature range 300 K to 16 K using picosecond pulses from the free electron laser at Stanford University. In addition, the first vibrational population relaxation measurements spanning a temperature range that takes a system from a liquid to a supercooled liquid to a glass are reported.
An account is given of the first infrared vibrational photon echo experiments conducted in liquids and a glasses. The experiments were performed on the CO stretching mode of the solute tungsten hexacarbonyl (W(CO)6) at approximately 5.05 micrometers (approximately 1980 cm-1) in the solvents 2-methytetrahydrofuran, and 2-methylpentane (2-MP). In 2-MP, it was possible to observe the photon echo decay at room temperature and follow the temperature dependence from room temperature to 10 K. The photon echo experiments were conducted using the Stanford superconducting-linear-accelerator-pumped Free Electron Laser as the source of tunable ps infrared pulses.
The influence of the environment on vibrational dynamics, and especially on the vibrational dephasing time, is investigated for a simple system : DCl in a van der Waals solid (N2 lattice). Photon echo experiments are performed using the infrared free electron laser CLIO. In solid nitrogen, decay times of the third order polarization are in the picosecond range. In the case of the isolated DCl monomers in van der Waals interaction with the host, the observed signals are interpreted in term of a rapid spectral diffusion. The two different stretching modes of DCl dimers, perturbed in a different way by the weak hydrogen bond, exhibit different coherence times, reflecting the influence of the interaction strength between the molecules.