Does the Adam-Gibbs relation hold in simulated supercooled liquids?

Abstract

We perform stringent tests of thermodynamic theories of the glass transition over the experimentally relevant temperature regime for several simulated glass-formers. The swap Monte Carlo algorithm is used to estimate the configurational entropy and static point-to-set lengthscale, and careful extrapolations are used for the relaxation times. We first quantify the relation between configurational entropy and the point-to-set lengthscale in two and three dimensions. We then show that the Adam-Gibbs relation is generally violated in simulated models for the experimentally relevant time window. Collecting experimental data for several supercooled molecular liquids, we show that the same trends are observed experimentally. Deviations from the Adam-Gibbs relation remain compatible with random first order transition theory, and may account for the reported discrepancies between Kauzmann and Vogel-Fulcher-Tammann temperatures. Alternatively, they may also indicate that even near $T_g$ thermodynamics is not the only driving force for slow dynamics.

arXiv comment13 pages, 8 figures

References in corpus (60)

• Theoretical perspective on the glass transition and amorphous materials
• Direct experimental evidence of a growing length scale accompanying the glass transition
• Theory of Structural Glasses and Supercooled Liquids
• The relationship between fragility, configurational entropy and the potential energy landscape of glass forming liquids
• Dynamics on the Way to Forming Glass: Bubbles in Space-time
• On the Adam-Gibbs-Wolynes scenario for the viscosity increase in glasses
• Inherent Structure Entropy of Supercooled Liquids
• Fragile-to-strong transition and polyamorphism in the energy landscape of liquid silica
• The frustration-based approach of supercooled liquids and the glass transition: a review and critical assessment
• Thermodynamic signature of growing amorphous order in glass-forming liquids
• Bond orientational ordering in liquids: Towards a unified description of water-like anomalies, liquid-liquid transition, glass transition, and crystallization
• Models and algorithms for the next generation of glass transition studies
• Glass and Jamming Transitions: From Exact Results to Finite-Dimensional Descriptions
• Growing length and time scales in glass forming liquids
• The Relationship of Dynamical Heterogeneity to the Adam-Gibbs and Random First-Order Transition Theories of Glass Formation
• Glassy Aging Dynamics
• Phase diagram of glassy systems in an external field
• The glass transition of dense fluids of hard and compressible spheres
• Broadband Dielectric Spectroscopy on Glass-Forming Propylene Carbonate
• Equilibrium sampling of hard spheres up to the jamming density and beyond
• Fundamental differences between glassy dynamics in two and three dimensions
• The Monte-Carlo dynamics of a binary Lennard-Jones glass-forming mixture
• Growing point-to-set length scale correlates with growing relaxation times in model supercooled liquids
• Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling
• Perspective: Configurational entropy of glass-forming liquids
• Dynamics and Configurational Entropy in the LW Model for Supercooled Orthoterphenyl
• Zero-temperature glass transition in two dimensions
• Corresponding States of Structural Glass Formers. II
• A brief critique of the Adam-Gibbs entropy model
• Specific Heats Cp, Cv, Cconf. and energy landscapes of glassforming liquids
• Does a growing static length scale control the glass transition?
• Efficient swap algorithms for molecular dynamics simulations of equilibrium supercooled liquids
• The excess wing in the dielectric loss of glass-forming ethanol: A relaxation process
• From boiling point to glass transition temperature: transport coefficients in molecular liquids follow three-parameter scaling
• The role of structure and entropy in determining differences in dynamics for glass formers with different interaction potentials
• Computing the Absolute Gibbs Free Energy in Atomistic Simulations: Applications to Defects in Solids
• Evaluation of configurational entropy of a model liquid from computer simulations
• Theory of the Structural Glass Transition: A Pedagogical Review
• The Static Lengthscale Characterizing the Glass Transition at Lower Temperatures
• A novel approach to numerical measurements of the configurational entropy in supercooled liquids
• The race to the bottom: approaching the ideal glass?
• Numerical determination of the exponents controlling the relationship between time, length and temperature in glass-forming liquids
• The Adam-Gibbs relation for glass-forming liquids in 2, 3 and 4 dimensions
• Point-to-set lengths, local structure, and glassiness
• Mean field theory of the swap Monte Carlo algorithm
• Dynamic relaxation of a liquid cavity under amorphous boundary conditions
• Atomistic structural mechanism for the glass transition: Entropic contribution
• Evidence of growing spatial correlations during the aging of glassy glycerol
• Length scale dependence of the Stokes-Einstein and Adam-Gibbs relations in model glass formers
• First steps of a nucleation theory in disordered systems
• Dynamic and thermodynamic crossover scenarios in the Kob-Andersen mixture: Insights from multi-CPU and multi-GPU simulations
• Efficient measurement of point-to-set correlations and overlap fluctuations in glass-forming liquids
• Does the configurational entropy of polydisperse particles exist?
• Configurational entropy of polydisperse supercooled liquids
• Surface tension fluctuations and a new spinodal point in glass-forming liquids
• Growing Surface Tension of Amorphous-Amorphous Interfaces on Approaching the Colloidal Glass Transition
• Bypassing sluggishness: SWAP algorithm and glassiness in high dimensions
• Activated dynamic scaling in the random-field Ising model: a nonperturbative functional renormalization group approach
• Diffusivity and configurational entropy maxima in short range attractive colloids
• Splitting up entropy into vibrational and configurational contributions in bulk metallic glasses: A thermodynamic approach

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