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The Journal of Chemical Physics

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

S. Saikan, Takakazu Nakabayashi, Yasuo Kanematsu, A. Imaoka

Published Oct 15, 1988• 18 citations
Publisher

Abstract

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).

DOI
10.1063/1.454801

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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.

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Physical review. B, Condensed matter•Feb 1, 1992•16 citations
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).
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 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.
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 signals of both primary and stimulated femtosecond photon echoes are observed and investigated in a dye-doped polymer film at room temperature using a modernized femtosecond echo-spectrometer. It should be noted that stimulated photon echo in the solid-state sample is observed for the first time at such a high temperature. Experimentally obtained decay curves of these signals have a nonexponential character. The spectra of these echo signals are also measured. It is found that the spectrum of the primary photon echo is short-wave shifted with respect to the spectrum of excitation. This can be used for the coherent laser cooling of a sample. The spectrum of the stimulated photon echo is also shifted to the short-wave range relative to the spectrum of excitation, but its shift is much less than that of the primary photon echo. The experiment shows that the femtosecond echo signals at room temperature are excited via the phonon-side band of the absorption line.
The signals of primary and stimulated femtosecond photon echo in polymer films doped with dye (phthalocyanine) molecules have been experimentally investigated at room temperature. A femtosecond echo spectrometer for these echo experiments is described. The decay curves of echo signals with increasing time intervals between excitation femtosecond pulses are obtained and blue shifts of the spectra of femtosecond echo signals with respect to the spectrum of excitation pulses are revealed. The possibilities of using the studied doped polymer films as recording media for high-temperature echo processors and coolants in optical refrigerators are analyzed.
The temperature-dependent femtosecond dephasing of vibronic lines of a dye, Nile blue, doped in a polymer (polyvinyl alcohol) was studied by using an incoherent-photon-echo technique. It is, to our knowledge, the first detailed study on temperature-dependent dephasing for vibronic lines in a dye-doped polymer system. Photon echoes for the vibronic lines displayed an exponential decay with the dephasing times less than 100 fs, and the temperature dependence of the dephasing was found to follow a power law of T1.5{\mathit{T}}^{1.5}T1.5 in the temperature range from 9.5 to 130 K. By comparing the results with the behavior of the zero-phonon line, we discuss the effect of the interactions with so-called two-level tunneling system and phonons in the polymer host on the femtosecond dephasing of the vibronic lines.