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Temperature-dependent spectral hole-burning study of dye–surface and mixed matrix–dye–surface systems

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Abstract

Temperature-dependent persistent spectral hole-burning measurements are reported on the dye–surface system Quinizarin/γ-alumina (Q/γ-Al2O3) and on the mixed matrix–dye–surface systems 3-methylpentane/Q/γ-Al2O3, methylene chloride/Q/γ-Al2O3, and n-heptane/Q/γ-Al2O3. In all cases the temperature dependence of the hole-burning linewidth ΓHB could be best fitted to a combination of a Tα law and a contribution from an exponentially activated process, indicating that the dynamics of the mixed systems are similar to Q/γ-Al2O3. For Q/γ-Al2O3 the power-law term shows clearly the glasslike nature of the γ-Al2O3 surface. The temperature dependence of ΓHB yielded a large coupling constant for the exponentially activated term for n-heptane/Q/γ-Al2O3, indicating a higher degree of crystallinity for the maxtrix n-heptane than for methylene chloride. The mixed matrix–dye–surface systems generally exhibit a smaller contribution of two-level-system modes to exponentially activated processes than does Q/γ-Al2O3. The distance from the zero-phonon line peak to the phonon side-hole peak ν˜0 differs by a factor of 3, demonstrating a distinct dependence of the dominant low-frequency mode on the chromophore environment. A very large ν˜0 of ≈50 cm−1 was found for the dye–surface system Q/γ-Al2O3. ν˜0 does not correlate to the frequency of the exponentially activated process. For Q/γ-Al2O3 stable holes could be burned even at 77 K. The Debye–Waller factor was measured for this system over an extended temperature range.

© 1992 Optical Society of America

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