Distribution of local relaxation events in an aging 3D glass: spatio-temporal correlation and dynamical heterogeneity

Abstract

We investigate the spatio-temporal distribution of microscopic relaxation events, defined through particle hops, in a model polymer glass using molecular dynamics simulations. We introduce an efficient algorithm to directly identify hops during the simulation, which allows the creation of a map of relaxation events for the whole system. Based on this map, we present density-density correlations between hops and directly extract correlation scales. These scales define collaboratively rearranging groups of particles and their size distributions are presented as a function of temperature and age. Dynamical heterogeneity is spatially resolved as the aggregation of hops into clusters, and we analyze their volume distribution and growth during aging. A direct comparison with the four-point dynamical susceptibility {\chi}4 reveals the formation of a single dominating cluster prior to the {\chi}4 peak, which indicates maximally correlated dynamics. An analysis of the fractal dimension of the hop clusters finds slightly non-compact shapes in excellent agreement with independent estimates from four-point correlations.