Depleting states dictate the ideal glass and physics of glass transition

TL;DR

This study uses advanced simulation techniques to explore the potential energy landscape of a 2D glass former, revealing the physical significance of the ideal glass and its relation to the entropy crisis across various system sizes and temperatures.

Contribution

It combines Swap Monte Carlo with PEL analysis to characterize the ideal glass and its properties in equilibrium, providing new insights into the entropy crisis and the fragile-to-strong transition.

Findings

Identification of a system size matching the macroscopic limit.

Quantification of the potential energy landscape down to the global minimum.

Observation of the fragile to strong transition and the ideal glass regime.

Abstract

Understanding the properties of supercooled fluids in equilibrium, even below the calorimetric glass transition $T_g$, is an elusive challenge. This is even more true for the properties of the ideal glass, defined as the minimum of the potential energy landscape (PEL) in the non-crystalline regime. Although its existence is a mathematical necessity due to the finite range of energies, its properties, and physical relevance are still undecided. Here we combine the million-fold acceleration of Swap Monte Carlo with PEL analysis to study a non-network 2D model glass former in equilibrium for a wide range of system sizes and temperatures. We observe the transition from fragile to strong behavior and provide a generic perspective to such observations in many experimental non-network glass formers, or the saturation of structural disorder upon cooling. Furthermore, we can identify a particular system size that shows quantitative agreement with the macroscopic limit, while allowing a complete characterization of the potential energy landscape (PEL) down to its global minimum. This implies the availability of configurational entropy down to the zero temperature limit without the detour via liquid entropy, thereby quantifying the putative entropy crisis. Through appropriate system size analysis, we can identify a low-energy depletion regime, including the ideal glass, and reveal its physical relevance for equilibrium properties over a wide temperature range, including below $T_g$.