Geometrical properties of the potential energy of the soft-sphere binary mixture

We report a detailed study of the stationary points (zero-force points) of the potential energy surface (PES) of a model structural glassformer. We compare stationary points found with two different algorithms (eigenvector following and square gradient minimization), and show that the mapping between instantaneous configuration and stationary points defined by those algorithms is as different as to strongly influence the instability index K vs. temperature plot, which relevance in analyzing the liquid dynamics is thus questioned. On the other hand, the plot of K vs. energy is much less sensitive to the algorithm employed, showing that the energy is the good variable to discuss geometric properties of the PES. We find new evidence of a geometric transition between a minima-dominated phase and a saddle-point-dominated one. We analyze the distances between instantaneous configurations and stationary points, and find that above the glass transition, the system is closer to saddle points than to minima

Glass and polycrystal states in a lattice spin model

We numerically study a nondisordered lattice spin system with a first order liquid-crystal transition, as a model for supercooled liquids and glasses. Below the melting temperature the system can be kept in the metastable liquid phase, and it displays a dynamic phenomenology analogous to fragile supercooled liquids, with stretched exponential relaxation, power law increase of the relaxation time and high fragility index. At an effective spinodal temperature Tsp the relaxation time exceeds the crystal nucleation time, and the supercooled liquid loses stability. Below Tsp liquid properties cannot be extrapolated, in line with Kauzmann's scenario of a `lower metastability limit' of supercooled liquids as a solution of Kauzmann's paradox. The off-equilibrium dynamics below Tsp corresponds to fast nucleation of small, but stable, crystal droplets, followed by extremely slow growth, due to the presence of pinning energy barriers. In the early time region, which is longer the lower the temperature, this crystal-growth phase is indistinguishable from an off-equilibrium glass, both from a structural and a dynamical point of view: crystal growth has not advanced enough to be structurally detectable, and a violation of the fluctuation-dissipation theorem (FDT) typical of structural glasses is observed. On the other hand, for longer times crystallization reaches a threshold beyond which crystal domains are easily identified, and FDT violation becomes compatible with ordinary domain growth.Comment: 25 page

An intermediate state between the kagome-ice and the fully polarized state in Dy2_2Ti2_2O7_7

Dy$_2$Ti$_2$O$_7$ is at present the cleanest example of a spin-ice material. Previous theoretical and experimental work on the first-order transition between the kagome-ice and the fully polarized state has been taken as a validation for the dipolar spin-ice model. Here we investigate in further depth this phase transition using ac-susceptibility and dc-magnetization, and compare this results with Monte-Carlo simulations and previous magnetization and specific heat measurements. We find signatures of an intermediate state between the kagome-ice and full polarization. This signatures are absent in current theoretical models used to describe spin-ice materials.Comment: 7 pages, 4 figure

Specific heat anomaly in a supercooled liquid with amorphous boundary conditions

We study the specific heat of a model supercooled liquid confined in a spherical cavity with amorphous boundary conditions. We find the equilibrium specific heat has a cavity-size-dependent peak as a function of temperature. The cavity allows us to perform a finite-size scaling (FSS) analysis, which indicates that the peak persists at a finite temperature in the thermodynamic limit. We attempt to collapse the data onto a FSS curve according to different theoretical scenarios, obtaining reasonable results in two cases: a "not-so-simple" liquid with nonstandard values of the exponents {\alpha} and {\nu}, and random first-order theory, with two different length scales.Comment: Includes Supplemental Materia

Response to "Comment on Static correlations functions and domain walls in glass-forming liquids: The case of a sandwich geometry" [J. Chem. Phys. 144, 227101 (2016)]

The point-to-set correlation function has proved to be a very valuable tool to probe structural correlations in disordered systems, but more than that, its detailed behavior has been used to try to draw information on the mechanisms leading to glassy behavior in supercooled liquids. For this reason it is of primary importance to discern which of those details are peculiar to glassy systems, and which are general features of confinement. Within the present response we provide an answer to the concerns raised in [J. Chem. Phys. 144, 227101 (2016)]

Dynamic relaxation of a liquid cavity under amorphous boundary conditions

The growth of cooperatively rearranging regions was invoked long ago by Adam and Gibbs to explain the slowing down of glass-forming liquids. The lack of knowledge about the nature of the growing order, though, complicates the definition of an appropriate correlation function. One option is the point-to-set correlation function, which measures the spatial span of the influence of amorphous boundary conditions on a confined system. By using a swap Monte Carlo algorithm we measure the equilibration time of a liquid droplet bounded by amorphous boundary conditions in a model glass-former at low temperature, and we show that the cavity relaxation time increases with the size of the droplet, saturating to the bulk value when the droplet outgrows the point-to-set correlation length. This fact supports the idea that the point-to-set correlation length is the natural size of the cooperatively rearranging regions. On the other hand, the cavity relaxation time computed by a standard, nonswap dynamics, has the opposite behavior, showing a very steep increase when the cavity size is decreased. We try to reconcile this difference by discussing the possible hybridization between MCT and activated processes, and by introducing a new kind of amorphous boundary conditions, inspired by the concept of frozen external state as an alternative to the commonly used frozen external configuration.Comment: Completely rewritten version. After the first submission it was realized that swap and nonswap dynamics results are qualitatively different. This version reports the results of both dynamics and discusses the different behaviors. 17 pages, 18 figure

A phase-separation perspective on dynamic heterogeneities in glass-forming liquids

We study dynamic heterogeneities in a model glass-former whose overlap with a reference configuration is constrained to a fixed value. The system phase-separates into regions of small and large overlap, so that dynamical correlations remain strong even for asymptotic times. We calculate an appropriate thermodynamic potential and find evidence of a Maxwell's construction consistent with a spinodal decomposition of two phases. Our results suggest that dynamic heterogeneities are the expression of an ephemeral phase-separating regime ruled by a finite surface tension