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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Time-resolved photon echo and fluorescence anisotropy study of organically doped sol-gel glasses

Eric L. Chronister, Drew M. L'Esperance, John M. Pelo, John Middleton, Robert A. Crowell

Published Dec 1, 1991• 1 citation
Publisher

Abstract

We present the first time resolved photon echo measurements of homogeneous dephasing of organic dopants in an inorganic sol-gel glass and compare these results with recent hole- burning experiments. In addition, energy transfer mechanisms and chromophore spatial distributions are investigated by time-resolved fluorescence anisotropy measurements.

DOI
10.1117/12.50657

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We present the first time resolved photon echo measurements of homogeneous dephasing of organic dopants in an inorganic sol-gel glass and compare these results with recent hole- burning experiments. In addition, energy transfer mechanisms and chromophore spatial distributions are investigated by time-resolved fluorescence anisotropy measurements.
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.
The range of relaxation rates present in amorphous systems is shown to affect the results of optical dephasing measurements. The interpretation of these experiments in terms of four-time correlation functions is introduced. Photon echo and hole burning results are shown for resorufin in three glass hosts: ethanol, d-ethanol, and glycerol. The hole burning data are shown to be affected by slow relaxation processes whereas the echo results are not. The implications of a slowest relaxation rate in amorphous systems are also considered.
Picosecond photon echo (PE) experiments are used to examine the optical dephasing and intermolecular interactions of organic chromophores in a variety of glassy organic and polymer hosts. The inherent disorder in these systems leads to dynamics which span times from picoseconds to hours and longer. The temperature dependent optical dephasing as measured by the PE follows a power law characteristic of tunnelling twolevel systems (TLS) at low temperatures (1 °K to 4 °K) and is exponentially activated at higher temperatures due to dephasing by additional modes. The nature of these modes will be addressed. These data and those from other line narrowing experiments such as hole burning allow the study both of fast dephasing processes and spectral diffusion due to slow fluctuations in the host. The observed lineshapes and holewidths require dipolar coupling between the chromophore and TLS and offer information on the distribution of relaxation rates. Furthermore, techniques sensitive to different timescales are used to examine host dynamics by removing the guest-host coupling from consideration. The data are discussed in conjunction with recently developed theoretical treatments of dephasing in disordered systems.
Temperature-dependent (1.2–2.1 K) photon echo measurements have been performed on quinizarin and rhodamine 101 doped into aluminosilica sol-gel glasses as well as rhodamine 101 doped poly-methyl-methacrylate (PMMA) polymer. We observe a temperature-dependent homogeneous linewidth for both quinizarin and rhodamine in the aluminosilica xerogel (ASX) matrix proportional to T2, in contrast to the T1.3±0.1 linewidth dependence typically observed for a variety of organic and inorganic glass hosts in this temperature range (including rhodamine 101 doped PMMA). The contrasting optical dephasing results for the ASX glass and PMMA suggest that the ASX glass may have unique two-level-system dynamics.