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Journal of the Optical Society of America B

Ultrafast dephasing of Resorufin in d-ethanol glass from 17 to 40 K studied by incoherent photon echo

N.V. Gruzdev, Силькис Эммануил Гершович, V. D. Titov, Yu. G. Vainer

Published Jun 1, 1992• 17 citations
Publisher

Abstract

The temperature dependence of the electronic dephasing of Resorufin in d-ethanol glass was measured from 1.7 to 40 K by incoherent photon echo (IPE) techniques. At T = 8–11 K good agreement between IPE and two-pulse picosecond photon echo (PPE) results was observed. For T < 8 K, PPE and IPE results differed; the difference is attributed to spectral diffusion on a nanosecond time scale. IPE results for T > 11 K confirm the hypothesis that high-temperature dephasing in this system is due mainly to interaction with a pseudolocal mode.

DOI
10.1364/josab.9.000941

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Chemical Physics Letters•Nov 1, 1988•49 citations
The temperature dependence of the electronic dephasing of Resorufin in d-ethanol glass was measured from 1.7 to 40 K by incoherent photon echo (IPE) techniques. At T = 8–11 K good agreement between IPE and two-pulse picosecond photon echo (PPE) results was observed. For T < 8 K, PPE and IPE results differed; the difference is attributed to spectral diffusion on a nanosecond time scale. IPE results for T > 11 K confirm the hypothesis that high-temperature dephasing in this system is due mainly to interaction with a pseudolocal mode.
The principles of incoherent photon echoes (IPE) are shortly recalled. The results on dynamics in doped organic glasses and polymers (resorufin in d‐ and d6‐ethanol and terrylene in polyethylene) studied by IPE are presented. In all cases the fast dephasing processes are related to coupling with both two‐level systems (TLS) and pseudolocal mode. The nanosecond spectral diffusion (SD) processes has been observed. The IPE‐results are compared with hole‐burning and single molecule spectroscopy (SMS) data.
The first two-pulse photon echo experiments on a chromophore in an organic glass are reported. The homogeneous electronic dephasing of resorufin in ethanol glass is measured from 1.5–11.4 K. The temperature dependence of the dephasing time does not fit the power law frequently predicted by theory for the dephasing characteristic of glasses. However, the temperature dependence can be accounted for by including dephasing from librations or acoustic phonons, mechanisms known to be important in crystals. The dephasing decay is found to be a single exponential for over six factors of e. The dephasing is also shown to be uncorrelated with the extent of nonphotochemical hole burning (NPHB). However, the homogeneous linewidth deduced from the photon echo is four times narrower than the linewidth obtained from NPHB, demonstrating that the hole is broadened by additional processes.
Photon echo and non-photochemical hole burning experiments on cresyl violet in ethanol glass are reported. At 1.5 K the optical dephasing time measured by the picosecond echo is eight times longer than the time measured by hole burning because of the difference in the time scales associated with the measurements. The observed temperature dependence arises from the glass's two-level systems and from a pseudolocal phonon mode at higher temperatures. Comparing the ratios of the echo to hole burning dephasing times for cresyl violet and resornfin, suggests that their dephasing is influenced by the nature of their ethanol solvation shells in addition to the dynamics of the bulk ethanol.