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Journal de Physique IV (Proceedings)

PHOTON-ECHO STUDY OF ULTRAFAST DEPHASING IN AMORPHOUS SOLIDS IN WIDE TEMPERATURE REGION WITH INCOHERENT LIGHT

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

Published Dec 1, 1991• 1 citation
Publisher

Abstract

The temperature-dependence of the electronic dephasing for resorufin in d-ethanol glass was measured from 1.7 to 35 K by incoherent photon echo. The difference between two-pulse picosecond photon echo and incoherent photon echo results was obtained and attributed to spectral diffusion in nanosecond time scale.
DOI
10.1051/jp4:19917117

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Journal of Luminescence•Oct 1, 1993•9 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 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.
Until now, in spite of a great number of experimental and theoretical works in study of organic amorphous solids, the basic features of the low temperature dynamics of these mediums are poorly understood. One of the main reason of this is the lack of experimental information about these dynamical processes. In particular, it’s necessary to learn more about optical dephasing in doped organic glasses and polymers for wider temperature interval. It will allow to test the existent theories more correctly and to create new conceptions.
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.