Anomalous diffusion in heterogeneous glass-forming liquids: Temperature-dependent behavior

Abstract

In a preceding paper, Mukhopadhyay and I studied the diffusive motion of a tagged molecule in a heterogeneous glass-forming liquid at temperatures just above a glass transition. Among other features of this system, we postulated a relation between heterogeneity and stretched-exponential decay of correlations, and we also confirmed that systems of this kind generally exhibit non-Gaussian diffusion on intermediate length and time scales. Here I extend this analysis to higher temperatures approaching the point where the heterogeneities disappear and thermal activation barriers become small. I start by modifying the continuous-time random-walk theory proposed earlier, and supplement this analysis with an extension of the excitation-chain theory of glass dynamics. I also use a key result from the shear-transformation-zone theory of viscous deformation of amorphous materials. Elements of each of these theories are then used to interpret experimental data for ortho-terphenyl, specifially, the diffusion and viscosity coefficients and neutron scattering measurements of the self intermediate scattering function. Reconciling the theory with these data sets provides insights about the crossover between super-Arrhenius and Arrhenius dynamics, length scales of spatial heterogeneities, violation of the Stokes-Einstein relation in glass-forming liquids, and the origin of stretched exponential decay of correlations.

12 pages, 7 figures

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• Realizing split-pulse x-ray photon correlation spectroscopy to measure ultrafast dynamics in complex matter