Three-state structural heterogeneity in a model two dimensional fluid

Abstract

Three structural populations with distinct average mobility are identified within an equilibrium two-dimensional Lennard-Jones fluid simulated via molecular dynamics at a constant temperature and varying density. Quantifying the structure of the immediate neighborhood of particles by a tessellation allows us to identify three distinct structural states by the shapes of the tessellation cells. Irrespective of dynamic particle exchange among these populations, each is observed to maintain their own thermodynamic and average dynamic properties across the liquid-solid transition. We expect these findings to be valuable for better understanding the structural basis of dynamical heterogeneity in complex fluids defined in terms of local mobility fluctuations.