Distribution of local relaxation events in an aging three-dimensional glass: Spatiotemporal correlation and dynamical heterogeneity

Publication Type
Journal Article
Year of Publication
Smessaert, Anton
Rottler, Jörg
Name of Publication
Physical Review E
Date Published

We investigate the spatiotemporal 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 χ4 reveals the formation of a single dominating cluster prior to the χ4 peak, which indicates maximally correlated dynamics. An analysis of the fractal dimension of the hop clusters finds slightly noncompact shapes in excellent agreement with independent estimates from four-point correlations.