Quantifying Structural Dynamic Heterogeneity in a Dense Two-dimensional Equilibrium Liquid

TL;DR

This study uses molecular dynamics simulations to classify local particle structures in a 2D Lennard-Jones fluid, revealing how structural heterogeneity correlates with dynamics across phases.

Contribution

It introduces a solid-angle tessellation method to identify and analyze distinct local structural classes in a 2D equilibrium liquid and solid.

Findings

Pentagonal neighborhoods dominate in the liquid phase.

Hexagonal neighborhoods dominate in the solid phase.

Clusters of different structures grow and percolate with changing density.

Abstract

We investigate the local structural fluctuations of a model equilibrium fluid with an aim of better understanding the structural basis of locally heterogeneous dynamics identified in recent simulations and experimental studies of glass-forming liquids and other strongly interacting particle systems, such as, lipid membranes, dusty plasmas, interfacial dynamics of crystals, internal dynamics of proteins, etc. In particular, we study a two-dimensional single component Lennard-Jones over a range of densities and constant temperature covering both the liquid and crystalline phase by molecular dynamics simulation. We identify three distinct structural classes of particles by examining the immediate neighborhood of individual particles based on a solid-angle based tessellation technique. In particular, the area distribution of the neighborhoods reveals cages having hexagonal, pentagonal and square symmetries. Pentagonal cells appear to be predominant motif in the liquid phase, while the solid phase is dominated by hexagonal cells, as in the case of the perfect crystal. Examining the spatial organization of particles belonging to each structural class separately shows that finite-size clusters formed by particles of hexagonal and pentagonal population found within liquids and solids, respectively, grow in a complementary way as a function of density and both particle populations percolate within liquid-crystal coexistence regime. Interestingly, the populations of particles with different local structures, defined by the arrangement of neighboring particles, are found to maintain different diffusivity computed from the velocity autocorrelation of constituent particles for all densities studied. Our analysis provides a new approach for analyzing and a possible framework for understanding the structural changes in soft materials.