Modern computational studies of the glass transition

Abstract

The physics of the glass transition and amorphous materials continues to attract the attention of a wide research community after decades of effort. Supercooled liquids and glasses have been studied numerically since the advent of molecular dynamics and Monte Carlo simulations, and computer studies have greatly enhanced both experimental discoveries and theoretical developments. In this Review, we provide a modern perspective on this area. We describe the need to go beyond canonical methods when studying the glass transition — a problem that is notoriously difficult in terms of timescales, length scales and physical observables. We summarize recent algorithmic developments to achieve enhanced sampling and faster equilibration by using replica-exchange methods, cluster and swap Monte Carlo algorithms, and other techniques. We then review some major advances afforded by these tools regarding the statistical mechanical description of the liquid-to-glass transition, and the mechanical, vibrational and thermal properties of the glassy solid. Computer simulations may unlock crucial aspects of how a liquid transforms into a glass, but are hampered by rapidly growing relaxation times near the transition. This Review summarizes progress towards overcoming this problem and creating realistic in silico glasses, and discusses what understanding has been enabled.