Structure factor realizability reveals the glass-dynamics onset temperature

TL;DR

This study reveals that the onset of glass dynamics correlates with a topological change in the structure factor realizability landscape, detectable through optimization difficulty, despite smooth structural changes.

Contribution

It introduces a novel approach linking the glass-dynamics onset to a topological transition in the structure factor realizability landscape, challenging previous notions.

Findings

Difficulty in generating target structure factors increases below the onset temperature.

A kink in the optimization error indicates the glass-dynamics onset.

Results are based on simulations with Dzugutov interactions.

Abstract

When liquids are cooled rapidly, they bypass crystallization and instead enter a supercooled state and then a glass state. Previous studies have shown that the static structure factors of high-temperature liquids, supercooled liquids, and glasses exhibit only subtle differences, leading to the conclusion that the glass transition cannot be predicted solely from structure factor changes. Our research challenges this limitation. Specifically, we studied the difficulty of generating configurations corresponding to target structure factors using stochastic gradient descent optimizations. While such optimizations easily converge when targeting the structure factors of higher temperature liquids, the difficulty significantly increases for lower temperature liquids and glasses. By quantifying this difficulty through the mean squared error achieved, we found a kink at the onset temperature of glass dynamics. Our results suggest that the onset of glass dynamics can be explained by a topological change in the realizability landscape of the structure factor, even though the structure factor itself only changes smoothly. Our results are currently based on computer simulations using original and modified Dzugutov interactions, and future work will determine whether our theory is applicable to other glass-forming systems.