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Physical Review A

Interference effects in IR photon echo spectroscopy of liquid water

Sergey Yeremenko, Maxim S. Pshenichnikov, Douwe A. Wiersma

Published Feb 22, 2006• 27 citations
Publisher

Abstract

Heterodyne-detected transient grating experiments on the OH-stretch mode of HDO dissolved in ${\mathrm{D}}_{2}\mathrm{O}$ 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.

DOI
10.1103/physreva.73.021804

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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.
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.
A novel interference effect in transient four-wave mixing is demonstrated. The phenomenon is based on phase-controlled Liouville-space pathways interference and observed in the heterodyne-detected stimulated photon echo. Changing the phase difference between the first two excitation pulses from $\ensuremath{\pi}/2$ to 0 leads from no signal to maximum echo signal. A Brownian oscillator dynamical model is successfully used to analyze the effect and simulate the experimental data. The relation between this time-domain interference effect and dephasing-induced resonance in four-wave mixing spectroscopy is elaborated.
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.
The noise tenaciously appearing in the optically heterodyne detected (OHD) transient optical Kerr effect (OKE) o f simple molecular liquids is investigated. We show that, for liquid samples of interest to us, coherent coupling does exist and appears as noise when not properly resolved. The strength of coherent coupling relative to the OKE depends critically on the sample position, with respect to the beam waist of the probe laser, as well as the angle subtended by the pump and probe beams. When the optics alignment is optimized for the OKE against coherent coupling the OHD-OKE signal is found to increase linearly with the local oscillator strength; the coherent coupling signal also appears to increase though the trend is not clear-cut. PACS. 42.50.Md- Optical transient phenomena: quantum beats, photon echo, freeinduction decay, dephasings and revivals, optical nutation, and self-induced transparency. PACS. 78.47.+p- Time-resolved optical spectroscopies and other ultrafast optical measurements in condensed matter. I.
We demonstrate coherent control over interference between different Liouville-space pathways that describe the generation of the nonlinear optical polarization in a stimulated photon echo. This control was exercised by phase-locking of the excitation pulses and observed in the heterodyne detected echo signal. A theoretical analysis of the effect is presented and found to be in good agreement with the obtained results. The relation between this novel time-domain interference effect and the pressure-induced extra resonance in four-wave mixing spectroscopy is discussed.
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.