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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Picosecond infrared vibrational photon echoes and lifetime measurements using the Stanford superconducting-accelerator-pumped free-electron laser

M. D. Fayer, David A. Zimdars, Andrei Tokmakoff, Scott Chen, Scott R. Greenfield, T. I. Smith, H. Alan Schwettman

Published Jul 14, 1993• 0 citations
Publisher

Abstract

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.

DOI
10.1117/12.148031

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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.
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.
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.
A superconducting accelerator-pumped free-electron laser (SCA/FEL) is used to perform photon echo experiments on a near-IR dye molecule in a polymeric glass. The SCA/FEL produces Fourier-transform-limited picosecond pulses at a repetition rate of 11.8 MHz. Its wavelength is continuously tunable. The experiments are conducted at 0.776 μm by doubling the output of the SCA/FEL tuned to 1.55 μm. At this wavelength, the SCA/FEL is operated in a burst mode. The duration of the bursts (macropulses) is 2 ms with a repetition rate of 10 Hz. Each individual pulse (micropulse) has a length of 3.2 ps and is approximately 1 μJ in energy. In the experiment a number of single micropulses are selected from each macropulse. The doubling, stabilization, synchronization, single-pulse selection, and detection electronics are described. These are the first photon echo experiments and, to our knowledge, the first optical coherence experiments performed using a free-electron laser as a source.
Vibrational photon echo experiments were performed on the asymmetric CO stretching mode of tungsten hexacarbonyl in glassy dibutylphthalate as a function of temperature using sub-picosecond infrared pulses (1976 cm−1) from a free electron laser. The echo decays display pronounced beats and are bi-exponential. The beats and bi-exponential decays arise because the bandwith of the pulses exceed the vibrational anharmonicity, leading to the excitation and dephasing of a multilevel coherence. From the beat frequency, the anharmonicity is determined to be 14.7 cm−1. From the bi-exponential decay components, the temperature-dependent vibrational dephasing of both the v = 0 → 1 and v = 1 → 2 transitions are determined.
We report on picosecond coherent transient spectroscopy on the asymmetric stretching mode in $a\ensuremath{-}{\mathrm{SiO}}_{0.1}$ thin films using the Dutch free-electron laser FELIX. A fast 10-K lifetime of 2.8 ps is obtained using laser-induced transient grating spectroscopy. Its thermal behavior suggests relaxation into two accepting modes possibly via the symmetric stretch mode of the Si-O-Si complex. Two-pulse photon echo measurements reveal phase dynamics with both an excitation density and temperature dependence, suggesting the presence of nonequilibrium Si-Si phonons. The temperature-dependent component of the pure dephasing may be attributable to two-phonon elastic scattering. From the probe pulse diffraction efficiency, a value of the nonlinear refractive index has been determined to be ${n}_{2}=3.73\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}3}{\mathrm{cm}}^{2}/\mathrm{GW}.$