Abstract
Tackling the low-temperature fate of supercooled liquids is challenging because of the immense time scales involved, which prevent equilibration and lead to the operational glass transition. Relating glassy behavior to an underlying, thermodynamic phase transition is a long-standing open question in condensed matter physics. Like experiments, computer simulations are limited by the small time window over which a liquid can be equilibrated. Here, we address the challenge of low-temperature equilibration using trajectory sampling in a system undergoing a nonequilibrium phase transition. This transition occurs in trajectory space between the normal supercooled liquid and a glassy state rich in low-energy geometric motifs. Our results indicate that this transition might become accessible in equilibrium configurational space at a temperature close to the so-called Kauzmann temperature, and they provide a possible route to unify dynamical and thermodynamical theories of the glass transition.Received 22 March 2016DOI:https://doi.org/10.1103/PhysRevX.7.031028Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasGlass transitionPhysical SystemsGlassesLiquidsPolymers & Soft MatterStatistical Physics
Highlights
Statistical mechanics was firmly established more than a hundred years ago [1], simple liquids remain a persistent challenge when cooled to low temperatures
We show that the nonequilibrium phase transition appears to be bound from below, with a lower critical point Tc
By means of numerical simulations employing trajectory sampling, we have explored the connection between a dynamical phase transition and the low-temperature thermodynamics of a model atomistic glassformer
Summary
Statistical mechanics was firmly established more than a hundred years ago [1], simple liquids remain a persistent challenge when cooled to low temperatures. At some point (typically bypassing crystallization), the structural relaxation time τα exceeds the experimentally or numerically accessible time scale, and the liquid falls out of equilibrium into a dynamically arrested state called a glass. This so-called operational glass transition is protocol dependent and distinct from equilibrium thermodynamic phase transitions. The idea that at very low temperatures a genuine thermodynamic phase transition controls dynamic arrest has been around for a long time, starting with an observation by Kauzmann [4]: Extrapolating the configurational entropy of the liquid suggests that it should fall
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