Numerical Investigation of Glassy Dynamics in Low Density Systems

Vitrification in colloidal systems typically occurs at high densities driven by sharply varying, short-ranged interactions. The possibility of glassy behavior arising from smoothly varying, long-ranged particle interactions has received relatively little attention. Here we investigate the behavior of screened charged particles, and explicitly demonstrate that these systems exhibit glassy properties in the regime of low temperature and low density. Properties close to this low density (Wigner) glass transition share many features with their hard-sphere counterparts, but differ in quantitative aspects that may be accounted for via microscopic theoretical considerations.Comment: 4 pages, 4 figures, revised versio

Systematic characterization of thermodynamic and dynamical phase behavior in systems with short-ranged attraction

In this paper we demonstrate the feasibility and utility of an augmented version of the Gibbs ensemble Monte Carlo method for computing the phase behavior of systems with strong, extremely short-ranged attractions. For generic potential shapes, this approach allows for the investigation of narrower attractive widths than those previously reported. Direct comparison to previous self-consistent Ornstein-Zernike approximation calculations are made. A preliminary investigation of out-of-equilibrium behavior is also performed. Our results suggest that the recent observations of stable cluster phases in systems without long-ranged repulsions are intimately related to gas-crystal and metastable gas-liquid phase separation.Comment: 10 pages, 8 figure

Inhomogeneous Mode-Coupling Theory and Growing Dynamic Length in Supercooled Liquids

We extend Mode-Coupling Theory (MCT) to inhomogeneous situations, relevant for supercooled liquid in pores, close to a surface, or in an external field. We compute the response of the dynamical structure factor to a static inhomogeneous external potential and provide the first direct evidence that the standard formulation of MCT is associated with a diverging length scale. We find in particular that the so called ``cages'' are in fact extended objects. Although close to the transition the dynamic length grows as |T-T_c|^-1/4 in _both_ the beta and alpha regimes, our results suggest that the fractal dimension of correlated clusters is larger in the alpha regime. We also derive inhomogeneous MCT equations valid to second order in gradients.Comment: 4 page

Numerically Exact Long Time Behavior of Nonequilibrium Quantum Impurity Models

A Monte Carlo sampling of diagrammatic corrections to the non-crossing approximation is shown to provide numerically exact estimates of the long-time dynamics and steady state properties of nonequilibrium quantum impurity models. This `bold' expansion converges uniformly in time and significantly ameliorates the sign problem that has heretofore limited the power of real-time Monte Carlo approaches to strongly interacting real-time quantum problems. The new approach enables the study of previously intractable problems ranging from generic long time nonequilibrium transport characteristics in systems with large onsite repulsion to the direct description of spectral functions on the real frequency axis in Dynamical Mean Field Theory

Cooperativity Beyond Caging: Generalized Mode Coupling Theory

The validity of mode coupling theory (MCT) is restricted by an uncontrolled factorization approximation of density correlations. The factorization can be delayed and ultimately avoided, however, by explicitly including higher order correlations. We explore this approach within a microscopically motivated schematic model. Analytic tractability allows us to discuss in great detail the impact of factorization at arbitrary order, including the limit of avoided factorization. Our results indicate a coherent picture for the capabilities as well as limitations of MCT. Moreover, including higher order correlations systematically defers the transition and ultimately restores ergodicity. Power-law divergence of the relaxation time is then replaced by continuous but exponential growth.Comment: 4 pages, 2 figure

Mode coupling theory in the FDR-preserving field theory of interacting Brownian particles

We develop a renormalized perturbation theory for the dynamics of interacting Brownian particles, which preserves the fluctuation-dissipation relation order by order. We then show that the resulting one-loop theory gives a closed equation for the density correlation function, which is identical with that in the standard mode coupling theory.Comment: version to be published in Fast Track Communication in Journal of Physics A:Math. Theo

Spontaneous and induced dynamic correlations in glass-formers II: Model calculations and comparison to numerical simulations

We study in detail the predictions of various theoretical approaches, in particular mode-coupling theory (MCT) and kinetically constrained models (KCMs), concerning the time, temperature, and wavevector dependence of multi-point correlation functions that quantify the strength of both induced and spontaneous dynamical fluctuations. We also discuss the precise predictions of MCT concerning the statistical ensemble and microscopic dynamics dependence of these multi-point correlation functions. These predictions are compared to simulations of model fragile and strong glass-forming liquids. Overall, MCT fares quite well in the fragile case, in particular explaining the observed crucial role of the statistical ensemble and microscopic dynamics, while MCT predictions do not seem to hold in the strong case. KCMs provide a simplified framework for understanding how these multi-point correlation functions may encode dynamic correlations in glassy materials. However, our analysis highlights important unresolved questions concerning the application of KCMs to supercooled liquids.Comment: 23 pages, 12 fig

Understanding How Femtosecond Laser Waveguide Fabrication in Glasses Works

In order to understand the physical processes associated with fs-laser waveguide writing in glass, the effects of the laser repetition rate, the material composition and feature size were studied. The resulting material changes were observed by collecting Raman and fluorescence spectra with a confocal microscope. The guiding behavior of the waveguides was evaluated by measuring near field laser coupling profiles in combination with white light microscopy. Waveguides and Bragg gratings were fabricated in fused silica using pulse repetition rates from 1 kHz to 1 MHz and a wide range of scan speeds and pulse energies. Two types of fluorescence were detected in fused silica, depending on the fabrication conditions. Fluorescence from self trapped exciton (E{prime}{sub {delta}}) defects, centered at 550 nm, were dominant for conditions with low total doses, such as using a 1 kHz laser with a scan speed of 20 {micro}m/s and pulse energies less than 1 {micro}J. For higher doses a broad fluorescence band, centered at 650 nm, associated with non-bridging oxygen hole center (NBOHC) defects was observed. Far fewer NBOHC defects were formed with the 1 MHz laser than with the kHz lasers possibly due to annealing of the defects during writing. We also observed an increase in the intensity of the 605 cm{sup -1} Raman peak relative to the total Raman intensity, corresponding to an increase in the concentration of 3-membered rings for all writing conditions. The magnitude of this increase in waveguides fabricated with a 1 MHz laser was nearly twice that of waveguides fabricated with a 1 kHz laser. Additional waveguides were fabricated in soda lime silicate glasses to assess the effects of changing the glass composition. These waveguides formed around, not inside the exposed regions. This is distinctly different from fused silica in which the waveguides are inside the exposed regions. A comprehensive analysis of all the experimental results indicates that good waveguides are formed below the actual damage threshold of the glass. The rapid quenching model, which correlates the refractive index of the modified material to its cooling rate, explains the effect of composition on waveguide behavior

Dynamical heterogeneity in a glass forming ideal gas

We conduct a numerical study of the dynamical behavior of a system of three-dimensional crosses, particles that consist of three mutually perpendicular line segments rigidly joined at their midpoints. In an earlier study [W. van Ketel et al., Phys. Rev. Lett. 94, 135703 (2005)] we showed that this model has the structural properties of an ideal gas, yet the dynamical properties of a strong glass former. In the present paper we report an extensive study of the dynamical heterogeneities that appear in this system in the regime where glassy behavior sets in. On the one hand, we find that the propensity of a particle to diffuse is determined by the structure of its local environment. The local density around mobile particles is significantly less than the average density, but there is little clustering of mobile particles, and the clusters observed tend to be small. On the other hand, dynamical susceptibility results indicate that a large dynamical length scale develops even at moderate densities. This suggests that propensity and other mobility measures are an incomplete measure of dynamical length scales in this system.Comment: 11 pages, 7 figure

Nonlinear viscoelasticity of metastable complex fluids

Many metastable complex fluids such as colloidal glasses and gels show distinct nonlinear viscoelasticity with increasing oscillatory-strain amplitude; the storage modulus decreases monotonically as the strain amplitude increases whereas the loss modulus has a distinct peak before it decreases at larger strains. We present a qualitative argument to explain this ubiquitous behavior and use mode coupling theory (MCT) to confirm it. We compare theoretical predictions to the measured nonlinear viscoelasticity in a dense hard sphere colloidal suspensions; reasonable agreement is obtained. The argument given here can be used to obtain new information about linear viscoelasticity of metastable complex fluids from nonlinear strain measurements.Comment: 7 pages, 3 figures, accepted for publication in Europhys. Let