Dynamics in a tetrahedral network glassformer: Vibrations, network rearrangements, and diffusion

We perform molecular dynamics simulation on a tetrahedral network glassformer using a model for viscous SiO2 by Coslovich and Pastore [J. Phys.: Condens. Matter 21, 285107 (2009)]. In this system, Si and O particles form a random network at low temperature T. We attach an ellipsoid to each particle to represent its time-averaged vibration tensor. We then examine the anisotropic vibrations of Si and O, where the ellipsoid orientations are correlated with the network. The ellipsoids exhibit marked vibrational heterogeneity. The configuration changes occur as breakage and reorganization of the network, where only one or two particles undergo large jumps at each rearrangement leading to diffusion. To the time-correlation functions, however, the particles surrounding these largely displaced ones yield significantly T-dependent contributions, resulting in a weak violation of the Stokes-Einstein relation. This crossover is mild in silica due to the small Si-O bond numbers per particle, while it is strong in fragile glassformers with large coordination numbers. On long timescales, jump events tend to occur in the same regions forming marked dynamic heterogeneity. We also calculate the diffusion constants and the viscosity. The diffusion obeys activation dynamics and may be studied by short-time analysis of irreversible jumps. (C) 2014 AIP Publishing LLC.