The Length Scales of Dynamic Heterogeneity: Results from Molecular Dynamics Simulations

TL;DR

This paper reviews how molecular dynamics simulations have advanced understanding of dynamic heterogeneities in liquids, revealing complex transient structures and cooperative behaviors crucial for amorphous material dynamics.

Contribution

It provides a comprehensive overview of the development of conceptual tools and kinetic length scales used to analyze dynamic heterogeneities in molecular simulations.

Findings

Identification of transient patches of rigidity and mobile tendrils

Development of new conceptual tools based on kinetic length scales

Insights into the relationship between structure and dynamics in amorphous materials

Abstract

Over times shorter than that required for relaxation of enthalpy, a liquid can exhibit striking heterogeneities. The picture of these heterogeneities is complex with transient patches of rigidity, irregular yet persistent, intersected by tendrils of mobile particles, flickering intermittently into new spatial patterns of motion and arrest. The study of these dynamic heterogeneities has, over the last 20 years, allowed us to characterize cooperative dynamics, to identify new strategies in controlling kinetics in glass-forming liquids and to begin to systematically explore the relationship between dynamics and structure that underpins the behaviour of amorphous materials. Computer simulations of the dynamics in atomic and molecular liquids have played a dominant role in all of this progress. While some may be uneasy about this reliance on modelling, it is unavoidable, given the amount of microscopic detail needed to characterize the dynamic heterogeneities. The complexities revealed by these simulations have called for new conceptual tools. In this essay, I have tried to provide the reader with a clear and complete account of how these tools have been developed in terms of the literature on kinetic length scales in molecular dynamics simulations. Through the `prism' of these length scales, this essay addresses the question what have we learnt about dynamic heterogeneities from computer simulations?