Journal of Chemical Physics, Vol.101, No.8, 6927-6943, 1994
Low-Temperature Dynamics in Amorphous Solids - A Photon-Echo Study
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.
Keywords:SPECTRAL-DIFFUSION DECAY;IMPURITY ELECTRONIC-TRANSITIONS;INDIVIDUAL 2-LEVEL SYSTEMS;DEPENDENT SPECIFIC-HEAT;RARE-EARTH IONS;THERMAL-CONDUCTIVITY;PICOSECOND PHOTON;ORGANIC GLASSES;VITREOUS SILICA;FAST GENERATION