A Double-Transition Scenario for Anomalous Diffusion in Glass-Forming Mixtures

We study by molecular dynamics computer simulation a binary soft-sphere mixture that shows a pronounced decoupling of the species' long-time dynamics. Anomalous, power-law-like diffusion of small particles arises, that can be understood as a precursor of a double-transition scenario, combining a glass transition and a separate small-particle localization transition. Switching off small-particle excluded-volume constraints slows down, rather than enhances, small-particle transport. The data are contrasted with results from the mode-coupling theory of the glass transition

The Dynamics of Silica Melts under High Pressure: Mode-Coupling Theory Results

The high-pressure dynamics of a computer-modeled silica melt is studied in the framework of the mode-coupling theory of the glass transition (MCT) using static-structure input from molecular-dynamics (MD) computer simulation. The theory reproduces the experimentally known viscosity minimum (diffusivity maximum) as a function of density or pressure and explains it in terms of a corresponding minimum in its critical temperature. This minimum arises from a gradual change in the equilibrium static structure which shifts from being dominated by tetrahedral ordering to showing the cageing known from high-density liquids. The theory is in qualitative agreement with computer simulation results.Comment: Presented at ESF EW Glassy Liquids under Pressure, to be published in Journal of Physic

Asymptotic analysis of mode-coupling theory of active nonlinear microrheology

We discuss a schematic model of mode-coupling theory for force-driven active nonlinear microrheology, where a single probe particle is pulled by a constant external force through a dense host medium. The model exhibits both a glass transition for the host, and a force-induced delocalization transition, where an initially localized probe inside the glassy host attains a nonvanishing steady-state velocity by locally melting the glass. Asymptotic expressions for the transient density correlation functions of the schematic model are derived, valid close to the transition points. There appear several nontrivial time scales relevant for the decay laws of the correlators. For the nonlinear friction coeffcient of the probe, the asymptotic expressions cause various regimes of power-law variation with the external force, and two-parameter scaling laws.Comment: 17 pages, 12 figure

Slow Dynamics in Ion-Conducting Sodium Silicate Melts: Simulation and Mode-Coupling Theory

A combination of molecular-dynamics (MD) computer simulation and mode-coupling theory (MCT) is used to elucidate the structure-dynamics relation in sodium-silicate melts (NSx) of varying sodium concentration. Using only the partial static structure factors from the MD as an input, MCT reproduces the large separation in relaxation time scales of the sodium and the silicon/oxygen components. This confirms the idea of sodium diffusion channels which are reflected by a prepeak in the static structure factors around 0.95 A^-1, and shows that it is possible to explain the fast sodium-ion dynamics peculiar to these mixtures using a microscopic theory.Comment: 4 pages, 4 figure

Sensitivity of arrest in mode-coupling glasses to low-q structure

We quantify, within mode coupling theory, how changes in the liquid structure affect that of the glass. Apart from the known sensitivity to the structure factor $S(q)$ at wavevectors around the first sharp diffraction peak $q_0$, we find a strong (and inverted) response to structure at wavevectors \emph{below} this peak: an increase in $S(q_0/2)$ {\em lowers} the degree of arrest over a wide $q$-range. This strong sensitivity to `caged cage' packing effects, on length scales of order 2d, is much weaker in attractive glasses where short-range bonding dominates the steric caging effect.Comment: 4 pages, 5 figures. v2: 3 figures replaced; text rewritte

Idealized glass transitions under pressure: dynamics versus thermodynamics

The interplay of slow dynamics and thermodynamic features of dense liquids is studied by examinining how the glass transition changes depending on the presence or absence of Lennard-Jones-like attractions. Quite different thermodynamic behavior leaves the dynamics unchanged, with important consequences for high-pressure experiments on glassy liquids. Numerical results are obtained within mode-coupling theory (MCT), but the qualitative features are argued to hold more generally. A simple square-well model can be used to explain generic features found in experiment.Comment: to be published in Phys. Rev. Let

Universal and non-universal features of glassy relaxation in propylene carbonate

It is demonstrated that the susceptibility spectra of supercooled propylene carbonate as measured by depolarized-light-scattering, dielectric-loss, and incoherent quasi-elastic neutron-scattering spectroscopy within the GHz window are simultaneously described by the solutions of a two-component schematic model of the mode-coupling theory (MCT) for the evolution of glassy dynamics. It is shown that the universal beta-relaxation-scaling laws, dealing with the asymptotic behavior of the MCT solutions, describe the qualitative features of the calculated spectra. But the non-universal corrections to the scaling laws render it impossible to achieve a complete quantitative description using only the leading-order-asymptotic results.Comment: 37 pages, 16 figures, to be published in Phys. Rev.

Colloidal gelation and non-ergodicity transitions

Within the framework of the mode coupling theory (MCT) of structural relaxation, mechanisms and properties of non-ergodicity transitions in rather dilute suspensions of colloidal particles characterized by strong short-ranged attractions are studied. Results building on the virial expansion for particles with hard cores and interacting via an attractive square well potential are presented, and their relevance to colloidal gelation is discussed.Comment: 10 pages, 4 figures; Talk at the Conference: "Unifying Concepts in Glass Physics" ICTP Trieste, September 1999; to be published in J. Phys.: Condens. Matte

Role of structural relaxations and vibrational excitations in the high-frequency dynamics of liquids and glasses

We present theoretical investigation on the high-frequency collective dynamics in liquids and glasses at microscopic length scales and terahertz frequency region based on the mode-coupling theory for ideal liquid-glass transition. We focus on recently investigated issues from inelastic-X-ray-scattering and computer-simulation studies for dynamic structure factors and longitudinal and transversal current spectra: the anomalous dispersion of the high-frequency sound velocity and the nature of the low-frequency excitation called the boson peak. It will be discussed how the sound mode interferes with other low-lying modes present in the system. Thereby, we provide a systematic explanation of the anomalous sound-velocity dispersion in systems -- ranging from high temperature liquid down to deep inside the glass state -- in terms of the contributions from the structural-relaxation processes and from vibrational excitations called the anomalous-oscillation peak (AOP). A possibility of observing negative dispersion -- the {\em decrease} of the sound velocity upon increase of the wave number -- is argued when the sound-velocity dispersion is dominated by the contribution from the vibrational dynamics. We also show that the low-frequency excitation, observable in both of the glass-state longitudinal and transversal current spectra at the same resonance frequency, is the manifestation of the AOP. As a consequence of the presence of the AOP in the transversal current spectra, it is predicted that the transversal sound velocity also exhibits the anomalous dispersion. These results of the theory are demonstrated for a model of the Lennard-Jones system.Comment: 25 pages, 22 figure

Dense colloidal suspensions under time-dependent shear

We consider the nonlinear rheology of dense colloidal suspensions under a time-dependent simple shear flow. Starting from the Smoluchowski equation for interacting Brownian particles advected by shearing (ignoring fluctuations in fluid velocity) we develop a formalism which enables the calculation of time-dependent, far-from-equilibrium averages. Taking shear-stress as an example we derive exactly a generalized Green-Kubo relation, and an equation of motion for the transient density correlator, involving a three-time memory function. Mode coupling approximations give a closed constitutive equation yielding the time-dependent stress for arbitrary shear rate history. We solve this equation numerically for the special case of a hard sphere glass subject to step-strain.Comment: 4 page