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Chemical Physics Letters

Host-dependent optical dephasing of dye molecules doped in cross-linked polyvinyl alcohols

Masaya Kawase, Shinya Fujiwara, Shunsuke Nakanishi, Hiroshi Itoh

Published Jul 1, 1992• 2 citations
Publisher
DOI
10.1016/0009-2614(92)86050-r

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Optical dephasing of the zero-phonon line (ZPL) of organic dye molecules doped in polyvinyl alcohol (PVA) and several cross-linked PVA derivatives was studied by using the incoherent photon echoes and the photophysical persistent hole-burning. It was found in the incoherent photon echo measurements that optical dephasing time of the ZPL increases with increasing the length of a cross-linker introduced to the PVA backbone. The difference in the temperature dependence of the dephasing time was also observed between a dye doped in PVA with and without the cross-link. When a longer cross-linker was introduced, the phonon sideband component in the incoherent photon echo signal became dominant in contrast to that in PVA with a relatively short cross-linker, while the dephasing time of the ZPL was still longer than that in PVA without the cross-link. Hole-burning studies showed that the phonon sideband spectrum of a dye doped in the cross-linked PVAs is essentially similar to that in PVA. However, the depth of the zero-phonon hole burnt with the same burning power was found to depend on the PVA hosts with the cross-linkers. These our findings suggest that the introduced cross-link does not alter the electron–phonon coupling modes or pseudo-local mode, but it drastically reduces the effect of the two-level tunneling systems in PVA on the optical dephasing of a doped dye. As a result, the dephasing time of the dye in the cross-linked PVAs becomes longer than that in PVA without the cross-link. The decrease of the optical dephasing by introducing the cross-link can be interpreted by assuming a void space in PVA, which is created near to the cross-linker. In addition, absorption and fluorescence spectra in these systems were measured, which imply the occurrence of weak dye–dye interaction when the dye is doped in PVA with a much longer cross-linker.

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Optical dephasing of the zero-phonon line (ZPL) of organic dye molecules doped in polyvinyl alcohol (PVA) and several cross-linked PVA derivatives was studied by using the incoherent photon echoes and the photophysical persistent hole-burning. It was found in the incoherent photon echo measurements that optical dephasing time of the ZPL increases with increasing the length of a cross-linker introduced to the PVA backbone. The difference in the temperature dependence of the dephasing time was also observed between a dye doped in PVA with and without the cross-link. When a longer cross-linker was introduced, the phonon sideband component in the incoherent photon echo signal became dominant in contrast to that in PVA with a relatively short cross-linker, while the dephasing time of the ZPL was still longer than that in PVA without the cross-link. Hole-burning studies showed that the phonon sideband spectrum of a dye doped in the cross-linked PVAs is essentially similar to that in PVA. However, the depth of the zero-phonon hole burnt with the same burning power was found to depend on the PVA hosts with the cross-linkers. These our findings suggest that the introduced cross-link does not alter the electron–phonon coupling modes or pseudo-local mode, but it drastically reduces the effect of the two-level tunneling systems in PVA on the optical dephasing of a doped dye. As a result, the dephasing time of the dye in the cross-linked PVAs becomes longer than that in PVA without the cross-link. The decrease of the optical dephasing by introducing the cross-link can be interpreted by assuming a void space in PVA, which is created near to the cross-linker. In addition, absorption and fluorescence spectra in these systems were measured, which imply the occurrence of weak dye–dye interaction when the dye is doped in PVA with a much longer cross-linker.
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.