Dynamic Model of Super-Arrhenius Relaxation Rates in Glassy Materials

We propose that the super-Arrhenius relaxation rates observed in glassy materials are determined by thermally nucleated rearrangements of increasing numbers of molecules at decreasing temperatures. In our model of this mechanism, string-like fluctuations in the neighborhood of shear transformation zones (STZ's) provide routes along which rearrangements can propagate, and the entropy associated with long enough strings allows the rearrangement energy to be distributed stably in the surrounding material. We further postulate that, at low enough temperatures, these fluctuations are localized on the interfaces between frustration-limited domains. Our result is a modified Vogel-Fulcher formula at low temperatures that crosses over to a simple Arrhenius law as the glass changes from being solid-like to liquid-like. To achieve agreement with experiment in the crossover region, we need to make what seem to us to be overly strong assumptions about the behavior of frustration-limited domains.

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