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Physical review. B, Condensed matter

Infrared transient grating and photon echo spectroscopy of oxygen vibrational modes in amorphous silicon thin films

Jon‐Paul R. Wells, Paul J. Phillips, Nicolae Tomozeiu, F.H.P.M. Habraken, J. I. Dijkhuis

Published Sep 29, 2003• 19 citations
Publisher

Abstract

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 ${n}_{2}=3.73\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}3}{\mathrm{cm}}^{2}/\mathrm{GW}.$

DOI
10.1103/physrevb.68.115207

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We report on picosecond coherent transient spectroscopy on the asymmetric stretching mode in a\ensuremath−SiO0.1a\ensuremath{-}{\mathrm{SiO}}_{0.1}a\ensuremath−SiO0.1​ 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 n2=3.73\ifmmode×\else\texttimes\fi10\ensuremath−3cm2/GW.{n}_{2}=3.73\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}3}{\mathrm{cm}}^{2}/\mathrm{GW}.n2​=3.73\ifmmode×\else\texttimes\fi10\ensuremath−3cm2/GW.
We present results of the first vibrational photon-echo, transient-grating, and temperature dependent transient-bleaching experiments on a-Si:H. Using these techniques, and the infrared light of a free electron laser, the vibrational population decay and phase relaxation of the Si-H stretching mode were investigated. Careful analysis of the data indicates that the vibrational energy relaxes directly into Si-H bending modes and Si phonons, with a distribution of rates determined by the amorphous host. Conversely, the pure dephasing appears to be single exponential, and can be modeled by dephasing via two-phonon interactions.
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.
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.
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.