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The Journal of Chemical Physics

Temperature-dependent optical dephasing in sol-gel glasses: Photon echo measurements of rhodamine 101 and quinizarin doped aluminosilica xerogels

Bruce J. Baer, Eric L. Chronister

Published Dec 8, 1995• 1 citation
Publisher

Abstract

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.

DOI
10.1063/1.469955

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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.
Picosecond photon echo experiments on rhodamine B and octadecyl rhodamine B in a PMMA matrix between 1.0 and 12.5 K are compared. The two dyes have identical first electronic excited state transitions but different masses and moments of inertia. Echo decay times are identical and individual decays at the same temperature from the two systems are superimposable. The high-temperature echo data can be fit to an activated process with an energy of 15 cm−1. We conclude that in this glassy matrix, high-temperature dephasing is caused by a mode of the host and not a mode of the guest as has been suggested for glasses and is common in crystals.
The integrated three-pulse photon echo signal of Nile blue doped in poly(methyl methacrylate) (PMMA) was measured two-dimensionally by varying the first coherence period and the subsequent population period. The electronic dephasing time was in the femtosecond time range even at low temperatures, whereas rephasing and echo formation were still possible even when the population period was extended to >100 ps. Oscillation was present in the echo signal even when population period was extended to longer values than the dephasing time of the vibrational coherence. Echo peak shift measurement indicated a presence of small spectral diffusion in the picosecond time range. A computer simulation was carried out from a model spectral density. The phonon mode of PMMA was represented by a Brownian oscillator centered at ∼116 cm -1, and it reproduced the temperature dependence of the echo signal surprisingly well.
The long-lived stimulated photon echo is put forward as a powerful technique to probe structural dynamics in glasses and other amorphous solids. We present results of optical dephasing measurements on several doped organic glasses (deuterated ethanol, toluene, and triethylamine) and polymers (polystyrene, polyvinylbutyral, and polymethylmethacrylate). Using a stochastic analysis within the so-called two-level-system model, we can extract from these measurements the distribution function of fluctuation rates over a huge range of time scales, varying from picoseconds to hundreds of milliseconds. We show that the dynamics, which lies at the origin of spectral diffusion, is very dependent on the glass structure and can be described by two separate hyperbolic distribution functions of fluctuation rates. From longitudinal photon echo measurements in the population dimension, we find evidence for structural dynamics which is not accounted for in the standard two-level-system model and which is related to a spatially inhomogeneous distribution of fluctuation centers.
A high-pressure photon echo study of the low-temperature dynamics of rhodamine 640 in a 2-methyltetrahydrofuran (2-MTHF) molecular glass is reported. High pressure is found to decrease the homogeneous dephasing rate comparably to the volume compression ratio. The pressured-induced line narrowing is also qualitatively similar to high-pressure hole burning results reported for a 2-MTHF glass doped with bacteriochlorophyll a . The results are consistent with a pressure-induced decrease in the number of tunneling two-level systems (TLSs) that may be associated with collapsible void space in the molecular glass. Comparable high-pressure photon echo studies of organic polymer glasses over the same low-temperature range do not show line narrowing at high pressure, suggesting an intrinsic difference in the nature of TLSs for molecular versus polymer glasses.
The homogeneous optical dephasing times (T2) and the non-photochemical hole burning (NPHB) linewidths of resorufin in glycerol glass are reported from 1.1 to 25.5 K. At low temperature, the linewidths obtained from NPHB are substantially wider than the linewidths (1/πT2) obtained from photon echo measurements, but the two become equal at high temperatures. The extra broadening of the NPHB is found to increase as T0.8. A model of homogeneous dephasing including both two-level system and pseudolocal mode contributions is successful over the entire temperature range.