Local-order fluctuations in Kob-Andersen-type glass formers

TL;DR

This paper introduces a novel statistical measure based on local order fluctuations to better understand structural relaxation in Kob-Andersen glass formers, revealing composition-independent behavior at the onset of glassy dynamics.

Contribution

It proposes using the variance of the extracopularity coefficient as a new way to characterize local order fluctuations in glass formers, linking it to glass-forming ability.

Findings

Fluctuation intensity is nearly composition independent at the onset temperature.

Decomposition of fluctuations into density and symmetry contributions.

Fluctuation intensity correlates with glass-forming ability.

Abstract

Notwithstanding decades of work, we still lack a satisfactory understanding of the structural relaxation that takes place as a liquid is rapidly cooled to form a glass. The present paper discusses a novel statistical characterization of this phenomenon in Kob-Andersen-type mixtures -- a simple yet powerful class of model glass formers. We use the variance of an order parameter called the extracopularity coefficient to measure the intensity of instantaneous fluctuations in local orientational order. This intensity is found to be nearly composition independent at the onset temperature of glassy dynamics for the standard Kob-Andersen mixture. We decompose these fluctuations into a density and symmetry contribution. Through the behavior of these contributions, we argue that the near composition independence prevails when the structure of the system equally resembles a liquid and a glass. We moreover report that the intensity of local-order fluctuations behaves like a heuristic measure of glass-forming ability, which could prove useful when exact methods are intractable.