Revisiting the slow dynamics of a silica melt using Monte Carlo simulations

We implement a standard Monte Carlo algorithm to study the slow, equilibrium dynamics of a silica melt in a wide temperature regime, from 6100 K down to 2750 K. We find that the average dynamical behaviour of the system is in quantitative agreement with results obtained from molecular dynamics simulations, at least in the long-time regime corresponding to the alpha-relaxation. By contrast, the strong thermal vibrations related to the Boson peak present at short times in molecular dynamics are efficiently suppressed by the Monte Carlo algorithm. This allows us to reconsider silica dynamics in the context of mode-coupling theory, because several shortcomings of the theory were previously attributed to thermal vibrations. A mode-coupling theory analysis of our data is qualitatively correct, but quantitative tests of the theory fail, raising doubts about the very existence of an avoided singularity in this system. We discuss the emergence of dynamic heterogeneity and report detailed measurements of a decoupling between translational diffusion and structural relaxation, and of a growing four-point dynamic susceptibility. Dynamic heterogeneity appears to be less pronounced than in more fragile glass-forming models, but not of a qualitatively different nature.Comment: 13 pages, 10 figures; to be published in Phys. Rev.

Numerical simulation of inductive heating processes

For product optimization regarding weight reduction, material properties have to be adapted efficiently. To achieve this, new compositions of materials can be created or the manufacturing process can be changed in a way that heterogeneous distributions of material properties are enabled. An example for such an improved process chain is the production of thermo-mechanically graded structures like shafts. The manufacturing method mainly consists of three stages. The first one is characterized by a local temperature increase of the workpiece due to inductive heating. In the second phase the workpiece is deformed and simultaneously cooled throughout the contact with the forming die. In the last step, however, a high pressured air stream is applied, leading to a partial cooling of the workpiece. The inductive heating step is controlled by an alternating current inducing a high frequency magnetic field, which causes a temperature increase due to the resulting eddy currents. To analyse this process, the coupling between the electric and the magnetic field is described by the fully coupled Maxwell equations. Moreover the heat conduction equation is considered to describe thermal effects. To solve this multifield the equations are in the first step decoupled using an additional time differentiation. In the second step an axisymmetric case is considered, motivated by the fact that the inductive heating process of a cylindrical shaft is analysed. Afterwards the resulting equations are spatially discretized by the Galerkin finite element method. The temporal discretization is carried out via the Newmark method so that afterwards the electrical source distribution can be achieved. As a consequence the temperature evolution is determined in a postprocessing step

Glassy dynamics in monodisperse hard ellipsoids

We present evidence from computer simulations for glassy dynamics in suspensions of monodisperse hard ellipsoids. In equilibrium, almost spherical ellipsoids show a first order transition from an isotropic phase to a rotator phase. When overcompressing the isotropic phase into the rotator regime, we observe super-Arrhenius slowing down of diffusion and relaxation, accompanied by two-step relaxation in positional and orientational correlators. The effects are strong enough for asymptotic laws of mode-coupling theory to apply. Glassy dynamics are unusual in monodisperse systems. Typically, polydispersity in size or a mixture of particle species is prerequisite to prevent crystallization. Here, we show that a slight particle anisometry acts as a sufficient source of disorder. This sheds new light on the question of which ingredients are required for glass formation.Comment: included data of prolate system in all figures and text, extended discussion of indicators of glassy dynamics, fixed symbol ambiguities, preprint forma

Glassy behaviour in a simple topological model

In this article we study a simple, purely topological, cellular model which is allowed to evolve through a Glauber-Kawasaki process. We find a non-thermodynamic transition to a glassy phase in which the energy (defined as the square of the local cell topological charge) fails to reach the equilibrium value below a characteristic temperature which is dependent on the cooling rate. We investigate a correlation function which exhibits aging behaviour, and follows a master curve in the stationary regime when time is rescaled by a factor of the relaxation time t_r. This master curve can be fitted by a von Schweidler law in the late beta-relaxation regime. The relaxation times can be well-fitted at all temperatures by an offset Arrhenius law. A power law can be fitted to an intermediate temperature regime; the exponent of the power law and the von Schweidler law roughly agree with the relationship predicted by Mode-coupling Theory. By defining a suitable response function, we find that the fluctuation-dissipation ratio is held until sometime later than the appearance of the plateaux; non-monotonicity of the response is observed after this ratio is broken, a feature which has been observed in other models with dynamics involving activated processes.Comment: 11 pages LaTeX; minor textual corrcetions, minor corrections to figs 4 & 7

A mode-coupling theory for the glassy dynamics of a diatomic probe molecule immersed in a simple liquid

Generalizing the mode-coupling theory for ideal liquid-glass transitions, equations of motion are derived for the correlation functions describing the glassy dynamics of a diatomic probe molecule immersed in a simple glass-forming system. The molecule is described in the interaction-site representation and the equations are solved for a dumbbell molecule consisting of two fused hard spheres in a hard-sphere system. The results for the molecule's arrested position in the glass state and the reorientational correlators for angular-momentum index $\ell = 1$ and $\ell = 2$ near the glass transition are compared with those obtained previously within a theory based on a tensor-density description of the molecule in order to demonstrate that the two approaches yield equivalent results. For strongly hindered reorientational motion, the dipole-relaxation spectra for the $\alpha$-process can be mapped on the dielectric-loss spectra of glycerol if a rescaling is performed according to a suggestion by Dixon et al. [Phys. Rev. Lett. {\bf 65}, 1108 (1990)]. It is demonstrated that the glassy dynamics is independent of the molecule's inertia parameters.Comment: 19 pages, 10 figures, Phys. Rev. E, in prin

Reorientational relaxation of a linear probe molecule in a simple glassy liquid

Within the mode-coupling theory (MCT) for the evolution of structural relaxation in glass-forming liquids, correlation functions and susceptibility spectra are calculated characterizing the rotational dynamics of a top-down symmetric dumbbell molecule, consisting of two fused hard spheres immersed in a hard-sphere system. It is found that for sufficiently large dumbbell elongations, the dynamics of the probe molecule follows the same universal glass-transition scenario as known from the MCT results of simple liquids. The $\alpha$-relaxation process of the angular-index-j=1 response is stronger, slower and less stretched than the one for j=2, in qualitative agreement with results found by dielectric-loss and depolarized-light-scattering spectroscopy for some supercooled liquids. For sufficiently small elongations, the reorientational relaxation occurs via large-angle flips, and the standard scenario for the glass-transition dynamics is modified for odd-j responses due to precursor phenomena of a nearby type-A MCT transition. In this case, a major part of the relaxation outside the transient regime is described qualitatively by the $\beta$-relaxation scaling laws, while the $\alpha$-relaxation scaling law is strongly disturbed.Comment: 40 pages. 10 figures as GIF-files, to be published in Phys. Rev.

The Debye-Waller factor of liquid silica: Theory and simulation

We show that the prediction of mode-coupling theory for a model of a network-forming strong glass-former correctly describes the wave-vector dependence of the Debye-Waller factor. To obtain a good description it is important to take into account the triplet correlation function c_3, which we evaluate from a computer simulation. Our results support the possibility that this theory is able to accurately describe the non-ergodicity parameters of simple as well as of network-forming liquids.Comment: 5 pages of Latex, 3 figure

The mean-squared displacement of a molecule moving in a glassy system

The mean-squared displacement (MSD) of a hard sphere and of a dumbbell molecule consisting of two fused hard spheres immersed in a dense hard-sphere system is calculated within the mode-coupling theory for ideal liquid-glass transitions. It is proven that the velocity correlator, which is the second time derivative of the MSD, is the negative of a completely monotone function for times within the structural-relaxation regime. The MSD is found to exhibit a large time interval for structural relaxation prior to the onset of the $\alpha$-process which cannot be described by the asymptotic formulas for the mode-coupling-theory-bifurcation dynamics. The $\alpha$-process for molecules with a large elongation is shown to exhibit an anomalously wide cross-over interval between the end of the von-Schweidler decay and the beginning of normal diffusion. The diffusivity of the molecule is predicted to vary non-monotonically as function of its elongation.Comment: 18 pages, 12 figures, Phys. Rev. E, in prin

Simulation study of Non-ergodicity Transitions: Gelation in Colloidal Systems with Short Range Attractions

Computer simulations were used to study the gel transition occurring in colloidal systems with short range attractions. A colloid-polymer mixture was modelled and the results were compared with mode coupling theory expectations and with the results for other systems (hard spheres and Lennard Jones). The self-intermediate scattering function and the mean squared displacement were used as the main dynamical quantities. Two different colloid packing fractions have been studied. For the lower packing fraction, $\alpha$-scaling holds and the wave-vector analysis of the correlation function shows that gelation is a regular non-ergodicity transition within MCT. The leading mechanism for this novel non-ergodicity transition is identified as bond formation caused by the short range attraction. The time scale and diffusion coefficient also show qualitatively the expected behaviour, although different exponents are found for the power-law divergences of these two quantities. The non-Gaussian parameter was also studied and very large correction to Gaussian behaviour found. The system with higher colloid packing fraction shows indications of a nearby high-order singularity, causing $\alpha$-scaling to fail, but the general expectations for non-ergodicity transitions still hold.Comment: 13 pages, 15 figure