Abstract
A universally accepted explanation for why liquids sometimes vitrify rather than crystallize remains hotly pursued, despite the ubiquity of glass in our everyday lives, the utilization of the glass transition in innumerable modern technologies, and nearly a century of theoretical and experimental investigation. Among the most compelling hypothesized mechanisms underlying glass formation is the development in the fluid phase of local structures that somehow prevent crystallization. Here, we explore that mechanism in the case of hard particle glasses by examining the glass transition in an extended alchemical (here, shape) space; that is, a space where particle shape is treated as a thermodynamic variable. We investigate simple systems of hard polyhedra, with no interactions aside from volume exclusion, and show via Monte Carlo simulation that glass formation in these systems arises from a multiplicity of competing local motifs, each of which is prevalent in—and predictable from—nearby ordered structures in alchemical space.
Highlights
A universally accepted explanation for why liquids sometimes vitrify rather than crystallize remains hotly pursued, despite the ubiquity of glass in our everyday lives, the utilization of the glass transition in innumerable modern technologies, and nearly a century of theoretical and experimental investigation
Our results show that the concept of alchemical space is a useful lens through which to understand the vitrification of hard particle fluids
Crystallization fails in these systems due to the presence of multiple local structures, each of which is preferred in crystals formed by particles nearby in shape space
Summary
A universally accepted explanation for why liquids sometimes vitrify rather than crystallize remains hotly pursued, despite the ubiquity of glass in our everyday lives, the utilization of the glass transition in innumerable modern technologies, and nearly a century of theoretical and experimental investigation. 1234567890():,; Fluids, upon rapid cooling or compression, may bypass crystallization and instead remain disordered, displaying relaxation times that grow by orders of magnitude over small density or temperature windows This fall out of equilibrium is widely known throughout the scientific community as the glass transition, and leveraged in many modern technologies including rewritable data storage devices[1] and fiber optic networks[2]. Prior works have considered individual systems, and argued that certain local structures arise in specific systems because they are preferred on a local length scale, but are prevented from growing and converting the liquid to a crystal because the structures are incommensurate with the embedding space[5,7,8,9], arrange themselves non-periodically[10,11,12,13,14], or are numerous in type and random in arrangement[15,16] These works, do not consider the system under investigation in the context of other closely-related systems. This local structural competition creates an ‘identity crisis’ in the fluid and promotes vitrification
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