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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Linear electron-phonon interaction in dye-doped polymers: Boson peak frequencies in polymers

S. Saikan

Published Jan 1, 1991• 0 citations

Abstract

This talk presents a review of our recent experimental results on femtosecond accumulated photon echo in dye-doped polymers. The aim of this research is to clarify the parameter that is most important in affecting seriously the linear electron-phonon coupling in these samples, and to find the materials which have extremely weak linear electron-phonon coupling. The latter research is needed for the improvement of the PHB memory materials. We have so far demonstrated experimentally that Fourier-transform spectroscopy [1] based on the femtosecond accumulated photon echo is most useful for these studies. Furthermore, the detection sensitivity for the accumulated photon echoes has been improved significantly with the use of the phase modulation technique [2].

DOI: 10.1364/pshb.1991.fd1

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The Journal of Chemical Physics•Oct 15, 1988•18 citations

This talk presents a review of our recent experimental results on femtosecond accumulated photon echo in dye-doped polymers. The aim of this research is to clarify the parameter that is most important in affecting seriously the linear electron-phonon coupling in these samples, and to find the materials which have extremely weak linear electron-phonon coupling. The latter research is needed for the improvement of the PHB memory materials. We have so far demonstrated experimentally that Fourier-transform spectroscopy [1] based on the femtosecond accumulated photon echo is most useful for these studies. Furthermore, the detection sensitivity for the accumulated photon echoes has been improved significantly with the use of the phase modulation technique [2].

Fourier-transform spectroscopy using the technique of femtosecond accumulated photon echo with incoherent light has been performed in dye-doped polymers. Several types of interference effect or quantum beat between the zero-phonon line and other spectral components including the phonon sideband, the vibronic lines, and the photoproduct state have been observed. Based on the density matrix incorporating the transition-frequency modulation, it is pointed out that the factorization approximation for the relaxation function holds rigorously in the accumulated photon echo. We also clarified that the Fourier cosine transform of the heterodyne-detected echo signal provides the hole-burning spectrum.

The temperature dependence of the Debye-Waller factor in dye-doped polymers has been investigated with femtosecond accumulated photon echo. The superiority of polyvinyl alcohol as the host polymer for the optical-memory material is ascribed to the higher phonon sideband frequency in this sample. It is pointed out that the temperature dependence of the Debye-Waller factor, in particular the phonon sideband frequency, is of fundamental importance to finding out the best polymer for high-temperature optical memory based on photochemical hole burning.

We study theoretically and experimentally the influence of a homogeneous static electric field on a photochemically accumulated stimulated photon echo in dye-doped polymers. The dependence of the time profile of the echo signal on the strength of the electric field is evaluated in the case of a linear Stark effect. Experiments using polymers doped with organic dye molecules are carried out at low temperature, and our new technique is applied to determine the difference of the permanent dipole moment in the ground and the first excited singlet electronic state of the impurity molecules.

It is reported about the first observation (in a solid-state sample) and detailed investigation of the stimulated femtosecond photon echo (SFPE) signals at room temperature in a polyvinylbutural film doped with molecules of phthalocyanine of HW 1009 type at the wavelength of 788 nm. A dependence of relative intensity of these echo-signals on time intervals between the second and the third exciting pulses was studied and the SFPE spectrum was investigated with respect to the spectra of both exciting pulses and signals of self-diffraction. It was found that the linear electron-phonon coupling is weak and the influence of the phonon-side band of the absorption line on the SFPE signals is less significantly than on the signals of primary photon echo.

Fourier-transform photon echo spectroscopy has been applied to the vibronic absorption band in dye molecule. The quantum beat between the vibronic lines has been observed in cresyl-violet and tetraphenyl-porphine doped in polymer films. The vibronic lines associated with the quantum beat have been identified with comparing the Fourier-transformed spectrum of the echo signal and the persistent hole-burning spectrum. The observed steep temperature dependence of the vibronic coherence has been discussed in comparison with the mild temperature dependence of vibrational coherence (sublevel coherence between vibronic states).