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Conference on Lasers and Electro-Optics Pacific Rim (CLEO-PR)

Charge transfer-like interaction between organic dyes and aromatic molecules doped in amorphous polymer detected by incoherent photon echoes

Hiroshi Itoh, Shunsuke Nakanishi, S. Furue, Keiko Isoda, Akinori Baba

Published Jan 20, 2003• 0 citations

Abstract

Relaxation processes of dye molecules doped in polymer hosts have been understood by various kinds of interaction, such as the dipole-dipole interaction between molecules, the interaction with the two-level systems (TLS) in the host polymer and the electron-phonon interaction. The study on these interactions has been conducted to search for new efficient materials for the photonic device such as, for example, an optical memory. We present how the charge-transfer (CT)-like interaction between a donor and an acceptor molecule affect the dephasing property in the dye/polymer system. The CT-like interaction has not been investigated in dye-doped polymer system so far. We detect the effect of the CT-like interaction by using a degenerate four-wave-mixing technique (photon echoes) since it can conveniently probe the weak interactions between molecules as the change of the polarization decay rate. The sample system we employed is the cresyl violet (CV) doped polymers (polyvinyl alcohol (PVA) and polymethyl methacrylate (PMMA)), to which the nitrobenzene molecules are introduced to induce the interaction with the CV molecule.

DOI: 10.1109/cleopr.1999.814672

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Relaxation processes of dye molecules doped in polymer hosts have been understood by various kinds of interaction, such as the dipole-dipole interaction between molecules, the interaction with the two-level systems (TLS) in the host polymer and the electron-phonon interaction. The study on these interactions has been conducted to search for new efficient materials for the photonic device such as, for example, an optical memory. We present how the charge-transfer (CT)-like interaction between a donor and an acceptor molecule affect the dephasing property in the dye/polymer system. The CT-like interaction has not been investigated in dye-doped polymer system so far. We detect the effect of the CT-like interaction by using a degenerate four-wave-mixing technique (photon echoes) since it can conveniently probe the weak interactions between molecules as the change of the polarization decay rate. The sample system we employed is the cresyl violet (CV) doped polymers (polyvinyl alcohol (PVA) and polymethyl methacrylate (PMMA)), to which the nitrobenzene molecules are introduced to induce the interaction with the CV molecule.

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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

{\mathit{T}}^{1.5}

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.

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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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.