Renewal events in glass-forming liquids

J Helfferich, EUROPEAN PHYSICAL JOURNAL E, 37, 73 (2014).

DOI: 10.1140/epje/i2014-14073-6

On cooling toward the glass transition temperature, glass-forming liquids display long periods of localized motion interrupted by fast "jumps" in the single-particle trajectories. Several theoretical models based on these single-particle jumps have been proposed, most prominently the continuous-time random walk (CTRW). The central assumption of the CTRW is that jumps are renewal events, i.e. that the internal clock of a particle can be reset upon a jump. In this paper, I present an easy-to-implement method to test whether jumps detected in a supercooled liquid or glass are renewal events or not. The test was applied to molecular dynamics simulations of a short-chain polymer melt, demonstrating that the jumps can in fact be treated as renewal events. The test further revealed that additional relaxation processes are present which are not accounted for in the CTRW picture, highlighting the limitations of this approach. The notion of renewal events in glass- forming systems could be a very important building block for the interpretation of aging and the glass transition. Furthermore, it could have practical implications for the study of non-equilibrium dynamics in glasses as well as mechanical rejuvenation.

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