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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Long-lived stimulated photon echo: the ideal probe of glass dynamics

Hans C. Meijers, Douwe A. Wiersma

Published Jan 1, 1992• 0 citations
Publisher

Abstract

In the last two decades the dynamics of glasses has been a field of great interest. In order to explain the dynamical properties of glasses the two-level-system model has been proposed. In this model an atom, or group of atoms, can access two potential minima separated by a barrier. Phonon-assisted-tunneling between the two minima of this asymmetric double well potential represents a jump between two different local glass structures. These double well potentials are referred to as two-level-systems (TLS). In the standard TLS-model the potentials do not change in time. The intrinsic disorder of the glass provides a wide range of asymmetries and a broad distribution of transition rates. Consequently the dynamics of the glass takes place over a broad range of time scales.

DOI
10.1364/shbl.1992.tha2

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In the last two decades the dynamics of glasses has been a field of great interest. In order to explain the dynamical properties of glasses the two-level-system model has been proposed. In this model an atom, or group of atoms, can access two potential minima separated by a barrier. Phonon-assisted-tunneling between the two minima of this asymmetric double well potential represents a jump between two different local glass structures. These double well potentials are referred to as two-level-systems (TLS). In the standard TLS-model the potentials do not change in time. The intrinsic disorder of the glass provides a wide range of asymmetries and a broad distribution of transition rates. Consequently the dynamics of the glass takes place over a broad range of time scales.
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 modified theoretical model of photon echoes (PE) in low-temperature doped glasses based on the tunneling two-level system (TLS) and stochastic sudden jump models has been developed. The distinguishing feature of the model is its adaptation for Monte Carlo technique. The developed approach is more general than usual PE theories and allows us to take into account the different microscopic parameters of spectral dynamics in doped amorphous solids: in particular, the minimal radius of interaction between TLS and chromophore molecules, the dispersion of this coupling constant, and the changes of matrix properties nearby chromophore (shell-effect). The developed theory was applied for calculations of two-pulse PE decays for an organic amorphous system with typical parameters. It was found that the slope of temperature dependence of the homogeneous line width is decreased with an increase in the above-mentioned minimal radius. This effect could be one of the main reasons for the discrepancy between some PE experimental results versus calculation using standard PE theory.
Recently in studies of fluorescence excitation and persistent spectral hole burning (PSHB) of single molecules in crystalline environment spectral jumps have been observed at 1.5 K providing new insights into the low temperature dynamics of the condensed phase [1]. The connection between PSHB and the phonon-induced dynamics in asymmetric double-well-potentials (DWP) has been used in a photophysical model of PSHB explaining also phonon detection by refilling of a spectral hole observed after irradiation with nanosecond heat pulses [2]. These DWP have been originally introduced in order to explain anomalous acoustic and thermal properties of amorphous materials by the socalled two-level systems, the existence of which is due to tunneling in DWP with appropriate parameters. The photophysical model is based on spectral shifts (matrix-shift-variations) caused by phonon-induced crossing of the barriers which can occur in all DWP if the phonon frequency is high enough.
The theory of optical photon echo and hole burning spectroscopies in low temperature glasses is discussed within the framework of the tunneling two-level system and stochastic sudden jump models. Exact results for the relevant theoretical quantities involve certain averages over the distributions of the two-level system energies and relaxation rates. The standard approximations for these averages are critically examined, for experimentally realistic parameters, via comparison to numerically exact calculations. The general conclusion is that the standard approximations are often used under conditions where they are not expected to be quantitatively accurate.