Point-to-set lengths, local structure, and glassiness

TL;DR

This paper extends the concept of point-to-set correlations to detect various types of structural order in glass-forming liquids, helping differentiate between critical ordering and glassiness, and providing a unified framework for understanding glass formation.

Contribution

It introduces a generalized definition of PTS correlations that captures any growing order, enabling clearer distinction between different mechanisms of slowing down in liquids.

Findings

Extended PTS correlations to detect local and amorphous order.

Provided a framework to distinguish critical ordering from glassiness.

Unified assessment of local versus amorphous order in glass formation.

Abstract

The growing sluggishness of glass-forming liquids is thought to be accompanied by growing structural order. The nature of such order, however, remains hotly debated. A decade ago, point-to-set (PTS) correlation lengths were proposed as measures of amorphous order in glass formers, but recent results raise doubts as to their generality. Here, we extend the definition of PTS correlations to agnostically capture any type of growing order in liquids, be it local or amorphous. This advance enables the formulation of a clear distinction between slowing down due to conventional critical ordering and that due to glassiness, and provides a unified framework to assess the relative importance of specific local order and generic amorphous order in glass formation.