Numerical investigation of the equilibrium Kauzmann transition in a two-dimensional atomistic glass

TL;DR

This study uses advanced Monte Carlo simulations to provide the first direct evidence of a Kauzmann transition in a two-dimensional atomistic glass, revealing a thermodynamic phase transition to an ideal glass state at zero temperature.

Contribution

It introduces a novel computational approach combining three Monte Carlo methods to explore the equilibrium properties of a 2D atomistic glass down to zero temperature, overcoming previous limitations.

Findings

Evidence of a Kauzmann transition at a temperature vanishing in the thermodynamic limit.

Confirmation of an ideal glass state with a hierarchical energy landscape.

First direct simulation-based demonstration of the bulk transition to a non-ergodic glass state.

Abstract

Dense liquids gradually transform into non-equilibrium amorphous solids as they pass through the experimental glass transition. Experimentally, ergodicity is lost because measurements are conducted within a finite time window. More than seventy years ago, Kauzmann posed a fundamental question: If experiments could run indefinitely, would there exist a critical temperature at which an ergodicity-breaking phase transition occurs? Random first-order transitions represent the modern theoretical framework for this idea, rigorously established in the mean-field limit of high-dimensional atomistic systems and several idealized physical models. However, achieving theoretical understanding in finite dimensions is challenging, while experimental and numerical limitations on accessible timescales hinder direct observation of the putative Kauzmann transition. Here, we overcome this longstanding barrier by developing a computational strategy that combines three advanced Monte Carlo methods to access the equilibrium thermodynamic properties of a two-dimensional atomistic glass-former down to zero temperature across a range of system sizes. This enables us to directly measure thermodynamic and structural observables that provide unambiguous evidence that the system undergoes a Kauzmann transition at a temperature that vanishes in the thermodynamic limit. This transition is towards an ideal glass state characterized by a complex energy landscape with a hierarchical organization of low-lying states. Our results are the first demonstration that computer simulations can fully probe the statistical mechanics of the bulk transition to a non-ergodic glass state. We anticipate that our study will serve as a foundation for future simulation work on larger systems, three-dimensional materials, and more complex glass-forming models to fully elucidate the nature of the glass state of matter.