Self-induced heterogeneity in deeply supercooled liquids

TL;DR

This paper uses computer simulations to analyze self-induced heterogeneity in deeply supercooled liquids, revealing broad fluctuations in thermodynamic and dynamic properties that correlate with slow dynamics near the glass transition.

Contribution

It provides a novel simulation-based analysis of self-induced heterogeneity, linking thermodynamic fluctuations to dynamic slowdowns in supercooled liquids.

Findings

Dynamic heterogeneity lifetimes match single molecule studies

Thermodynamic fluctuations are broader than expected

Fluctuations correlate with slow dynamics

Abstract

A theoretical treatment of deeply supercooled liquids is difficult because their properties emerge from spatial inhomogeneities that are self-induced, transient, and nanoscopic. I use computer simulations to analyse self-induced static and dynamic heterogeneity in equilibrium systems approaching the experimental glass transition. I characterise the broad sample-to-sample fluctuations of salient dynamic and thermodynamic properties in elementary mesoscopic systems. Findings regarding local lifetimes and distributions of dynamic heterogeneity are in excellent agreement with recent single molecule studies. Surprisingly broad thermodynamic fluctuations are also found, which correlate well with dynamics fluctuations, thus providing a local test of the thermodynamic origin of slow dynamics.