Perspective: Configurational entropy of glass-forming liquids
arXiv:1902.07679 · doi:10.1063/1.5091961
Abstract
The configurational entropy is one of the most important thermodynamic quantities characterizing supercooled liquids approaching the glass transition. Despite decades of experimental, theoretical, and computational investigation, a widely accepted definition of the configurational entropy is missing, its quantitative characterization remains fraud with difficulties, misconceptions and paradoxes, and its physical relevance is vividly debated. Motivated by recent computational progress, we offer a pedagogical perspective on the configurational entropy in glass-forming liquids. We first explain why the configurational entropy has become a key quantity to describe glassy materials, from early empirical observations to modern theoretical treatments. We explain why practical measurements necessarily require approximations that make its physical interpretation delicate. We then demonstrate that computer simulations have become an invaluable tool to obtain precise, non-ambiguous, and experimentally-relevant measurements of the configurational entropy. We describe a panel of available computational tools, offering for each method a critical discussion. This perspective should be useful to both experimentalists and theoreticians interested in glassy materials and complex systems.
20 pages, 11 figures
References in corpus (39)
- Theoretical perspective on the glass transition and amorphous materials
- Supercooled Liquids for Pedestrians
- Strong scaling of general-purpose molecular dynamics simulations on GPUs
- Probing the equilibrium dynamics of colloidal hard spheres above the mode-coupling glass transition
- Perspective: Highly stable vapor-deposited glasses
- Glassy Aging Dynamics
- Rigorous Inequalities between Length and Time Scales in Glassy Systems
- The glass transition of dense fluids of hard and compressible spheres
- Exact theory of dense amorphous hard spheres in high dimension. I. The free energy
- Mosaic multi-state scenario vs. one-state description of supercooled liquids
- Zero-temperature glass transition in two dimensions
- Do Binary Hard Disks Exhibit an Ideal Glass Transition?
- Finite size effects in the dynamics of glass-forming liquids
- Analytic determination of dynamical and mosaic length scales in a Kac glass model
- Efficient swap algorithms for molecular dynamics simulations of equilibrium supercooled liquids
- Calorimetric glass transition explained by hierarchical dynamic facilitation
- The role of structure and entropy in determining differences in dynamics for glass formers with different interaction potentials
- Tuning the fragility of a glassforming liquid by curving space
- The race to the bottom: approaching the ideal glass?
- Evidence for a disordered critical point in a glass-forming liquid
- Deconstructing the glass transition through critical experiments on colloids
- Can the glass transition be explained without a growing static length scale?
- Density controls the kinetic stability of ultrastable glasses
- Phase diagram of a polydisperse soft-spheres model for liquids and colloids
- Ideal glass states are not purely vibrational: Insight from randomly pinned glasses
- Dynamic and thermodynamic crossover scenarios in the Kob-Andersen mixture: Insights from multi-CPU and multi-GPU simulations
- Does the configurational entropy of polydisperse particles exist?
- Configurational entropy of polydisperse supercooled liquids
- Generalized entropy theory of glass-formation in fully flexible polymer melts
- Local order and crystallization of dense polydisperse hard spheres
- Supercooled liquids, the glass transition, and computer simulations
- Experimental Determination of Configurational Entropy in a Two-Dimensional Liquid under Random Pinning
- Random Field Ising-like effective theory of the glass transition II: Finite Dimensional Models
- Random-Field Ising like effective theory of the glass transition: I Mean-Field Models
- Diffusivity and configurational entropy maxima in short range attractive colloids
- Nonperturbative fluctuations and metastability in a simple model: from observables to microscopic theory and back
- Another resolution of the configurational entropy paradox as applied to hard spheres
- Effect of particle exchange on the glass transition of binary hard spheres
- Note: A replica liquid theory of binary mixtures
Cited by in corpus (38)
- Modern computational studies of the glass transition
- Colloidal Hard Spheres: Triumphs, Challenges and Mysteries
- Active glasses
- Polymer Glass Formation: Role of Activation Free Energy, Configurational Entropy, and Collective Motion
- Does the Adam-Gibbs relation hold in simulated supercooled liquids?
- Perspective: Gardner Physics in Amorphous Solids and Beyond
- Structure-dynamics relationships in cryogenically deformed bulk metallic glass
- Ultrastable metallic glasses in silico
- Self-induced heterogeneity in deeply supercooled liquids
- How to "measure" a structural relaxation time that is too long to be measured?
- Relaxation dynamics in the energy landscape of glass-forming liquids
- Statistical mechanics of coupled supercooled liquids in finite dimensions
- On the overlap between configurations in glassy liquids
- Splitting up entropy into vibrational and configurational contributions in bulk metallic glasses: A thermodynamic approach
- The Devil is in the details: Pentagonal bipyramids and dynamic arrest
- Monte Carlo simulations of glass-forming liquids beyond Metropolis
- Thermodynamics and its correlation with dynamics in a mean-field model and pinned systems: A comparative study using two different methods of entropy calculation
- Large heat-capacity jump in cooling-heating of fragile glass from kinetic Monte Carlo simulations based on a two-state picture
- Is glass a state of matter?
- Collective relaxation dynamics in a three-dimensional lattice glass model
- RFOT theory for glassy dynamics in a single condensed polymer
- Fragile-to-Strong Crossover, growing length scales, and dynamic heterogeneity in Wigner Glasses
- First-principles study on the specific heat of glass at glass transition with a case study on glycerol
- Selecting Relevant Structural Features for Glassy Dynamics by Information Imbalance
- When you can't count, sample! Computable entropies beyond equilibrium from basin volumes
- Emergence of cooperatively reorganizing cluster and super-Arrhenius dynamics of fragile supercooled liquids
- The Angell Plot from the Potential Energy Landscape Perspective
- A Generative Diffusion Model for Amorphous Materials
- Quotient Maps and Configuration Spaces of Hard Disks
- Entropy Multiparticle Correlation Expansion for a Crystal
- Computational Methods toward Ultrastable Glasses
- Mean-squared Energy Difference for Exploring Potential Energy Landscapes of Supercooled Liquids
- Terminal stage of highly viscous flow
- Rényi complexity in mean-field disordered systems
- Prigogine-Defay ratio of glassy freezing scales with liquid fragility
- Broadened phonon-assisted wide-band radiation and subsequent low-threshold self-absorption coherent modulation in the high-entropy glass system doped with Nd3+ ions
- Configurational Entropy of Self Propelled Glass Formers
- Static self-induced heterogeneity in glass-forming liquids: Overlap as a microscope