From ultra-fast growth to avalanche growth in devitrifying glasses

Abstract

During devitrification, pre-existing crystallites grow by adding particles to their surface via a process that is either thermally activated (diffusive mode) or happens without kinetic barriers (fast crystal growth mode). It is yet unclear what factors determine the crystal growth mode and how to predict it. With simulations of repulsive hard-sphere-like (Weeks–Chandler–Andersen) glasses, we show for the first time that the same system at the same volume fraction and temperature can devitrify via both modes depending on the preparation protocol of the glass. We prepare two types of glass: conventional glass (CG) via fast quenching and uniform glass (UG) via density homogenization. First, we bring either glass into contact with a crystal (X) and find the inherent structure (CGX/UGX). During energy minimization, the crystal front grows deep into the CG interface, while the growth is minimal for UG. When thermal noise is added, this behavior is reflected in different crystallization dynamics. CGX exhibits a density drop at the crystal growth front, which correlates with enhanced dynamics at the interface and a fast growth mode. This mechanism may explain the faster crystal growth observed below the glass transition experimentally. In contrast, UGX grows via intermittent avalanche-like dynamics localized at the interface, a combination of localized mechanical defects and the exceptional mechanical stability imposed by the UG glass phase.