Non-Equilibrium Phase Transition in an Atomistic Glassformer: the Connection to Thermodynamics

Abstract

Tackling the low-temperature fate of supercooled liquids is challenging due to the immense timescales involved, which prevent equilibration and lead to the operational glass transition. Relating glassy behaviour 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 provide a possible route to unify dynamical and thermodynamical theories of the glass transition.

accepted in Physical. Rev. X

References in corpus (19)

• Theoretical perspective on the glass transition and amorphous materials
• The large deviation approach to statistical mechanics
• Supercooled Liquids for Pedestrians
• Fractal free energy landscapes in structural glasses
• The role of local structure in dynamical arrest
• Identifying structural flow defects in disordered solids using machine learning methods
• Roles of icosahedral and crystal-like order in hard spheres glass transition
• Fifth-order susceptibility unveils growth of thermodynamic amorphous order in glass-formers
• Understanding fragility in supercooled Lennard-Jones mixtures. I. Locally preferred structures
• Equilibrium sampling of hard spheres up to the jamming density and beyond
• Equilibrium phase diagram of a randomly pinned glass-former
• Growing Dynamical Facilitation on Approaching the Random Pinning Colloidal Glass Transition
• Finite-temperature critical point of a glass transition
• Strong geometric frustration in model glassformers
• Evidence for a disordered critical point in a glass-forming liquid
• Experimental Evidence for a Structural-Dynamical Transition in Trajectory Space
• Statistical Mechanics and Dynamics of a 3-Dimensional Glass-Forming System
• Deformation of inherent structures to detect long-range correlations in supercooled liquids
• Recasting a model atomistic glassformer as a system of icosahedra

Cited by in corpus (32)

• A characteristic energy scale in glasses
• The race to the bottom: approaching the ideal glass?
• Real Space Analysis of Colloidal Gels: Triumphs, Challenges and Future Directions
• Classical density functional theory, unconstrained crystallization, and polymorphic behavior
• Phase transitions in fluctuations and their role in two-step nucleation
• Mechanical properties of simple computer glasses
• Dynamic facilitation theory: A statistical mechanics approach to dynamic arrest
• Scaling Description of Dynamical Heterogeneity and Avalanches of Relaxation in Glass-Forming Liquids
• Aging in thermal active glasses
• Experimental Determination of Configurational Entropy in a Two-Dimensional Liquid under Random Pinning
• Bypassing sluggishness: SWAP algorithm and glassiness in high dimensions
• Structural-dynamical transition in the Wahnström mixture
• Dynamical coexistence in moderately polydisperse hard-sphere glasses
• Diffusion coefficient power laws and defect-driven glassy dynamics in swap acceleration
• Stable glassy configurations of the Kob-Andersen model using swap Monte Carlo
• Classifying the age of a glass based on structural properties: A machine learning approach
• Modeling non-linear dielectric susceptibilities of supercooled molecular liquids
• Selecting Relevant Structural Features for Glassy Dynamics by Information Imbalance
• Exploring canyons in glassy energy landscapes using metadynamics
• Rejuvenation and memory effects in active glasses induced by thermal and active cycling
• Discovery of a paired Gaussian and long-tailed distribution of potential energies in nanoglasses
• Gauge invariance and hyperforce correlation theory for equilibrium fluid mixtures
• Dynamical phase transitions for the activity biased Ising model in a magnetic field
• A critical comparison of general-purpose collective variables for crystal nucleation
• Does mesoscopic elasticity control viscous slowing down in glassforming liquids?
• Computational Methods toward Ultrastable Glasses
• Interpretability of linear regression models of glassy dynamics
• Probing the Local Response of Glass-forming Liquids by Laser Excitations
• Configurational constraints on glass formation in the liquid calcium aluminate system
• Dynamical Phase Transitions and their Relation to Thermodynamic Glass Physics
• Unifying atoms and colloids near the glass transition through bond-order topology
• Isomorphs in nanoconfined liquids