Configurational Entropy and its Crisis in Metastable States: Ideal Glass Transition in a Dimer Model as a Paragidm of a Molecular Glass

TL;DR

This paper investigates the entropy crisis in metastable states of a dimer lattice model, revealing its role as the fundamental cause of the ideal glass transition in molecular systems.

Contribution

It introduces a lattice dimer model to analyze metastability and demonstrates the entropy crisis as the root of the ideal glass transition, linking microscopic interactions to macroscopic glassy behavior.

Findings

Existence of entropy crisis in metastable states

Entropy crisis underpins the ideal glass transition

Orientational interactions influence liquid-liquid transitions

Abstract

We discuss the need for discretization to evaluate the configurational entropy in a general model. We also discuss the prescription using restricted partition function formalism to study the stationary limit of metastable states. We introduce a lattice model of dimers as a paradigm of molecular fluid and study metastability in it to investigate the root cause of glassy behavior. We demonstrate the existence of the entropy crisis in metastable states, from which it follows that the entropy crisis is the root cause underlying the ideal glass transition in systems with particles of all sizes. The orientational interactions in the model control the nature of the liquid-liquid transition observed in recent years in molecular glasses.