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Physical review. B, Condensed matter

Fourier-transform spectroscopy in dye-doped polymers using the femtosecond accumulated photon echo

S. Saikan, Takakazu Nakabayashi, Yasuo Kanematsu, N. Tato

Published Oct 15, 1988• 67 citations
Publisher

Abstract

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.

DOI
10.1103/physrevb.38.7777

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Observation of vibronic quantum beat in dye-doped polymers using femtosecond accumulated photon echo

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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).

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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].

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Subpicosecond Photon Echo Quantum Beats in a Dye-Doped Polymer

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The temperature dependence of vibronic quantum beats in dye-doped polymer films has been investigated using femtosecond accumulated photon echoes. It has been found that the vibronic quantum beat is not discernible above liquid-nitrogen temperature. It makes a striking contrast with the previous observation of the quantum beat in transient pump-probe experiments performed at room temperature. Based on the density matrix incorporating the fluctuation of the transition frequency, it is pointed out that there is no contribution of sublevel coherence to the accumulated photon echo, and the line broadening of the vibronic state or phonon sideband obscures the quantum beat at higher temperature. On the other hand, in the transient pump-probe experiment, the quantum beat is caused by the sublevel coherence, as was previously pointed out by Mitsunaga and Tang [Phys. Rev. A 35, 1720 (1987)]. Hence it is concluded that the influence of the frequency fluctuation on the sublevel coherence is relatively small despite the serious line broadening of the vibronic state.

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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.

Physical review. B, Condensed matter•Feb 15, 1990•64 citations
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.
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).
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].
Subpicosecond photon echo quantum beats were studied in a dye, Rhodamine 800, doped in a polymer (polyvinyl alcohol) by using an incoherent photon echo technique. At the long-wavelength tail of absorption, photon echo quantum beats were observed as the sinusoidal modulation with the frequency of about 100 cm-1, which resulted from the interference between a single vibronic line and the zero-phonon line. The dephasing time of the vibronic line and its temperature dependence were briefly studied. At nearly the peak of absorption, the quantum beats appeared as more complicated modulation, indicating the contribution from multiple vibronic lines.
The temperature dependence of vibronic quantum beats in dye-doped polymer films has been investigated using femtosecond accumulated photon echoes. It has been found that the vibronic quantum beat is not discernible above liquid-nitrogen temperature. It makes a striking contrast with the previous observation of the quantum beat in transient pump-probe experiments performed at room temperature. Based on the density matrix incorporating the fluctuation of the transition frequency, it is pointed out that there is no contribution of sublevel coherence to the accumulated photon echo, and the line broadening of the vibronic state or phonon sideband obscures the quantum beat at higher temperature. On the other hand, in the transient pump-probe experiment, the quantum beat is caused by the sublevel coherence, as was previously pointed out by Mitsunaga and Tang [Phys. Rev. A 35, 1720 (1987)]. Hence it is concluded that the influence of the frequency fluctuation on the sublevel coherence is relatively small despite the serious line broadening of the vibronic state.
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.