Browsing by Author "Berthier, Ludovic"

Now showing 1 - 12 of 12
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    Breaking the glass ceiling: Configurational entropy measurements in extremely supercooled liquids
    (2017-06-01) Berthier, Ludovic; Charbonneau, Patrick; Coslovich, Daniele; Ninarello, Andrea; Ozawa, M; Yaida, Sho
    Liquids relax extremely slowly on approaching the glass state. One explanation is that an entropy crisis, due to the rarefaction of available states, makes it increasingly arduous to reach equilibrium in that regime. Validating this scenario is challenging, because experiments offer limited resolution, while numerical studies lag more than eight orders of magnitude behind experimentally-relevant timescales. In this work we not only close the colossal gap between experiments and simulations but manage to create in-silico configurations that have no experimental analog yet. Deploying a range of computational tools, we obtain four estimates of their configurational entropy. These measurements consistently confirm that the steep entropy decrease observed in experiments is found also in simulations even beyond the experimental glass transition. Our numerical results thus open a new observational window into the physics of glasses and reinforce the relevance of an entropy crisis for understanding their formation.
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    Bypassing sluggishness: SWAP algorithm and glassiness in high dimensions
    Berthier, Ludovic; Charbonneau, Patrick; Kundu, Joyjit
    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.
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    Configurational entropy measurements in extremely supercooled liquids that break the glass ceiling.
    (Proceedings of the National Academy of Sciences of the United States of America, 2017-10-10) Berthier, Ludovic; Charbonneau, Patrick; Coslovich, Daniele; Ninarello, Andrea; Ozawa, Misaki; Yaida, Sho
    Liquids relax extremely slowly on approaching the glass state. One explanation is that an entropy crisis, because of the rarefaction of available states, makes it increasingly arduous to reach equilibrium in that regime. Validating this scenario is challenging, because experiments offer limited resolution, while numerical studies lag more than eight orders of magnitude behind experimentally relevant timescales. In this work, we not only close the colossal gap between experiments and simulations but manage to create in silico configurations that have no experimental analog yet. Deploying a range of computational tools, we obtain four estimates of their configurational entropy. These measurements consistently confirm that the steep entropy decrease observed in experiments is also found in simulations, even beyond the experimental glass transition. Our numerical results thus extend the observational window into the physics of glasses and reinforce the relevance of an entropy crisis for understanding their formation.
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    Efficient measurement of point-to-set correlations and overlap fluctuations in glass-forming liquids.
    (J Chem Phys, 2016-01-14) Berthier, Ludovic; Charbonneau, Patrick; Yaida, Sho
    Cavity point-to-set correlations are real-space tools to detect the roughening of the free-energy landscape that accompanies the dynamical slowdown of glass-forming liquids. Measuring these correlations in model glass formers remains, however, a major computational challenge. Here, we develop a general parallel-tempering method that provides orders-of-magnitude improvement for sampling and equilibrating configurations within cavities. We apply this improved scheme to the canonical Kob-Andersen binary Lennard-Jones model for temperatures down to the mode-coupling theory crossover. Most significant improvements are noted for small cavities, which have thus far been the most difficult to study. This methodological advance also enables us to study a broader range of physical observables associated with thermodynamic fluctuations. We measure the probability distribution of overlap fluctuations in cavities, which displays a non-trivial temperature evolution. The corresponding overlap susceptibility is found to provide a robust quantitative estimate of the point-to-set length scale requiring no fitting. By resolving spatial fluctuations of the overlap in the cavity, we also obtain quantitative information about the geometry of overlap fluctuations. We can thus examine in detail how the penetration length as well as its fluctuations evolve with temperature and cavity size.
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    Finite Dimensional Vestige of Spinodal Criticality above the Dynamical Glass Transition.
    (Physical review letters, 2020-09) Berthier, Ludovic; Charbonneau, Patrick; Kundu, Joyjit
    Finite dimensional signatures of spinodal criticality are notoriously difficult to come by. The dynamical transition of glass-forming liquids, first described by mode-coupling theory, is a spinodal instability preempted by thermally activated processes that also limit how close the instability can be approached. We combine numerical tools to directly observe vestiges of the spinodal criticality in finite dimensional glass formers. We use the swap Monte Carlo algorithm to efficiently thermalize configurations beyond the mode-coupling crossover, and analyze their dynamics using a scheme to screen out activated processes, in spatial dimensions ranging from d=3 to d=10. We observe a strong softening of the mean-field square-root singularity in d=3 that is progressively restored as d increases above d=8, in surprisingly good agreement with perturbation theory.
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    Front-Mediated Melting of Isotropic Ultrastable Glasses.
    (Physical review letters, 2019-10) Flenner, Elijah; Berthier, Ludovic; Charbonneau, Patrick; Fullerton, Christopher J
    Ultrastable vapor-deposited glasses display uncommon material properties. Most remarkably, upon heating they are believed to melt via a liquid front that originates at the free surface and propagates over a mesoscopic crossover length, before crossing over to bulk melting. We combine swap Monte Carlo with molecular dynamics simulations to prepare and melt isotropic amorphous films of unprecedendtly high kinetic stability. We are able to directly observe both bulk and front melting, and the crossover between them. We measure the front velocity over a broad range of conditions, and a crossover length scale that grows to nearly 400 particle diameters in the regime accessible to simulations. Our results disentangle the relative roles of kinetic stability and vapor deposition in the physical properties of stable glasses.
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    Gardner physics in amorphous solids and beyond.
    (The Journal of chemical physics, 2019-07) Berthier, Ludovic; Biroli, Giulio; Charbonneau, Patrick; Corwin, Eric I; Franz, Silvio; Zamponi, Francesco
    One of the most remarkable predictions to emerge out of the exact infinite-dimensional solution of the glass problem is the Gardner transition. Although this transition was first theoretically proposed a generation ago for certain mean-field spin glass models, its materials relevance was only realized when a systematic effort to relate glass formation and jamming was undertaken. A number of nontrivial physical signatures associated with the Gardner transition have since been considered in various areas, from models of structural glasses to constraint satisfaction problems. This perspective surveys these recent advances and discusses the novel research opportunities that arise from them.
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    Growing timescales and lengthscales characterizing vibrations of amorphous solids.
    (Proc Natl Acad Sci U S A, 2016-07-26) Berthier, Ludovic; Charbonneau, Patrick; Jin, Yuliang; Parisi, Giorgio; Seoane, Beatriz; Zamponi, Francesco
    Low-temperature properties of crystalline solids can be understood using harmonic perturbations around a perfect lattice, as in Debye's theory. Low-temperature properties of amorphous solids, however, strongly depart from such descriptions, displaying enhanced transport, activated slow dynamics across energy barriers, excess vibrational modes with respect to Debye's theory (i.e., a boson peak), and complex irreversible responses to small mechanical deformations. These experimental observations indirectly suggest that the dynamics of amorphous solids becomes anomalous at low temperatures. Here, we present direct numerical evidence that vibrations change nature at a well-defined location deep inside the glass phase of a simple glass former. We provide a real-space description of this transition and of the rapidly growing time- and lengthscales that accompany it. Our results provide the seed for a universal understanding of low-temperature glass anomalies within the theoretical framework of the recently discovered Gardner phase transition.
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    How to create equilibrium vapor-deposited glasses
    (2017-08-23) Berthier, Ludovic; Charbonneau, Patrick; Flenner, E; Zamponi, Francesco
    Glass films created by vapor-depositing molecules onto a substrate can exhibit properties similar to those of ordinary glasses aged for thousands of years. It is believed that enhanced surface mobility is the mechanism that allows vapor deposition to create such exceptional glasses, but it is unclear how this effect is related to the final state of the film. Here we use molecular dynamics simulations to model vapor deposition and an efficient Monte Carlo algorithm to determine the deposition rate needed to create equilibrium glassy films. We obtain a scaling relation that quantitatively captures the efficiency gain of vapor deposition over bulk annealing, and demonstrates that surface relaxation plays the same role in the formation of vapor-deposited glasses as bulk relaxation in ordinary glass formation.
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    Origin of Ultrastability in Vapor-Deposited Glasses.
    (Physical review letters, 2017-11) Berthier, Ludovic; Charbonneau, Patrick; Flenner, Elijah; Zamponi, Francesco
    Glass films created by vapor-depositing molecules onto a substrate can exhibit properties similar to those of ordinary glasses aged for thousands of years. It is believed that enhanced surface mobility is the mechanism that allows vapor deposition to create such exceptional glasses, but it is unclear how this effect is related to the final state of the film. Here we use molecular dynamics simulations to model vapor deposition and an efficient Monte Carlo algorithm to determine the deposition rate needed to create ultrastable glassy films. We obtain a scaling relation that quantitatively captures the efficiency gain of vapor deposition over bulk annealing, and demonstrates that surface relaxation plays the same role in the formation of vapor-deposited glasses as bulk relaxation does in ordinary glass formation.
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    Point-to-set lengths, local structure, and glassiness.
    (Phys Rev E, 2016-09) Yaida, Sho; Berthier, Ludovic; Charbonneau, Patrick; Tarjus, Gilles
    The growing sluggishness of glass-forming liquids is thought to be accompanied by growing structural order. The nature of such order, however, remains hotly debated. A decade ago, point-to-set (PTS) correlation lengths were proposed as measures of amorphous order in glass formers, but recent results raise doubts as to their generality. Here, we extend the definition of PTS correlations to agnostically capture any type of growing order in liquids, be it local or amorphous. This advance enables the formulation of a clear distinction between slowing down due to conventional critical ordering and that due to glassiness, and provides a unified framework to assess the relative importance of specific local order and generic amorphous order in glass formation.
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    Zero-temperature glass transition in two dimensions
    Berthier, Ludovic; Charbonneau, Patrick; Ninarello, Andrea; Ozawa, Misaki; Yaida, Sho
    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.