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Ref Arxiv: 1902.07679
DOI: 10.1063/1.5091961
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13 Citations
Résumé:

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.

Commentaires: 20 pages, 11 figures, submitted to the Journal of Chemical Physics. Réf Journal: J. Chem. Phys. 150, 160902 (2019)

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Ref Arxiv: 1805.09035
DOI: 10.1038/s41467-019-09512-3
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16 Citations
Résumé:

The nature of the glass transition is theoretically understood in the mean-field limit of infinite spatial dimensions, but the problem remains totally open in physical dimensions. Nontrivial finite-dimensional fluctuations are hard to control analytically, and experiments fail to provide conclusive evidence regarding the nature of the glass transition. Here, we use Monte Carlo simulations that fully bypass the glassy slowdown, and access equilibrium states in two-dimensional glass-forming liquids at low enough temperatures to directly probe the transition. We find that the liquid state terminates at a thermodynamic glass transition at zero temperature, which is associated with an entropy crisis and a diverging static correlation length.

Commentaires: 23 pages, 18 figures. Réf Journal: Nat. Commun. 10, 1508 (2019)

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Ref Arxiv: 1810.10256
DOI: 10.1103/PhysRevX.9.011049
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9 Citations
Résumé:

We numerically analyse the landscape governing the evolution of the vibrational dynamics of hard disk glasses as the density increases towards jamming. We find that the dynamics becomes slow, spatially correlated, and starts to display aging dynamics across an avoided Gardner transition, with a phenomenology that resembles three dimensional observations. We carefully analyse the behaviour of single glass samples, and find that the emergence of aging dynamics is controlled by the apparition of a complex organisation of the landscape that splits into a remarkable hierarchy of minima as jamming is approached. Our results show that the mean-field prediction of a Gardner phase characterized by an ultrametric structure of the landscape provides a useful description of finite dimensional systems, even when the Gardner transition is avoided.

Ref HAL: hal-02082177_v1
Ref Arxiv: 1805.12378
DOI: 10.1063/1.5086509
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19 Citations
Résumé:

It was recently discovered that SWAP, a Monte Carlo algorithm that involves the exchange of pairs of particles of differing diameters, can dramatically accelerate the equilibration of simulated supercooled liquids in regimes where the normal dynamics is glassy. This spectacular effect was subsequently interpreted as direct evidence against a static, cooperative explanation of the glass transition such as the one offered by the random first-order transition (RFOT) theory. We review several empirical facts that support the opposite view, namely, that a local mechanism cannot explain the glass transition phenomenology. We explain the speedup induced by SWAP within the framework of the RFOT theory. We suggest that the efficiency of SWAP stems from a postponed onset of glassy dynamics, which allows the efficient exploration of configuration space even in the regime where the physical dynamics is dominated by activated events across free-energy barriers. We describe this effect in terms of `crumbling metastability' and use the example of nucleation to illustrate the possibility of circumventing free-energy barriers of thermodynamic origin by a change of the local dynamical rules.

Commentaires: 15 pages, 3 figures; v2: improved discussions and clarifications

Ref HAL: hal-02074910_v1
Ref Arxiv: 1810.06950
DOI: 10.1103/PhysRevE.99.031301
WoS: 000460663400001
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8 Citations
Résumé:

The recent implementation of a swap Monte Carlo algorithm (SWAP) for polydisperse mixtures fully bypasses computational sluggishness and closes the gap between experimental and simulation timescales in physical dimensions $d=2$ and $3$. Here, we consider suitably optimized systems in $d=2, 3,\dots, 8$, to obtain insights into the performance and underlying physics of SWAP. We show that the speedup obtained decays rapidly with increasing the dimension. SWAP nonetheless delays systematically the onset of the activated dynamics by an amount that remains finite in the limit $d \to \infty$. This shows that the glassy dynamics in high dimensions $d>3$ is now computationally accessible using SWAP, thus opening the door for the systematic consideration of finite-dimensional deviations from the mean-field description.

Commentaires: Réf Journal: Phys. Rev. E 99, 031301 (2019)

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Ref Arxiv: 1810.01213
DOI: 10.1103/PhysRevE.99.012107
WoS: WOS:000455062400003
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11 Citations
Résumé:

A novel form of amorphous matter characterized by marginal stability was recently discovered in the mean-field theory of structural glasses. Using this approach, we provide complete phase diagrams delimiting the location of the marginally stable glass phase for a large variety of pair interactions and physical conditions, extensively exploring physical regimes relevant to granular matter, foams, emulsions, hard and soft colloids, and molecular glasses. We find that all types of glasses may become marginally stable, but the extent of the marginally stable phase highly depends on the preparation protocol. Our results suggest that marginal phases should be observable for colloidal and non-Brownian particles near jamming and for poorly annealed glasses. For well-annealed glasses, two distinct marginal phases are predicted. Our study unifies previous results on marginal stability in mean-field models and will be useful to guide numerical simulations and experiments aimed at detecting marginal stability in finite-dimensional amorphous materials.

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Résumé:

How glasses break: A randomcritical point for yielding