Self-diffusion in sheared colloidal suspensions: violation of fluctuation-dissipation relation

Using memory-function formalism we show that in sheared colloidal suspensions the fluctuation-dissipation theorem for self-diffusion, i.e. Einstein's relation between self-diffusion and mobility tensors, is violated and propose a new way to measure this violation in Brownian Dynamics simulations. We derive mode-coupling expressions for the tagged particle friction tensor and for an effective, shear-rate dependent temperature

Dynamic glass transition: bridging the gap between mode-coupling theory and the replica approach

We clarify the relation between the ergodicity breaking transition predicted by mode-coupling theory and the so-called dynamic transition predicted by the static replica approach. Following Franz and Parisi [Phys. Rev. Lett. 79, 2486 (1997)], we consider a system of particles in a metastable state characterized by non-trivial correlations with a quenched configuration. We show that the assumption that in a metastable state particle currents vanish leads to an expression for the replica off-diagonal direct correlation function in terms of a replica off-diagonal static four-point correlation function. A factorization approximation for this function results in an approximate closure for the replica off-diagonal direct correlation function. The replica off-diagonal Ornstein-Zernicke equation combined with this closure coincides with the equation for the non-ergodicity parameter derived using the mode-coupling theory.Comment: revised version; to be published in EP

Gaussian density fluctuations, mode coupling theory, and all that

We consider a toy model for glassy dynamics of colloidal suspensions: a single Brownian particle diffusing among immobile obstacles. If Gaussian factorization of static density fluctuations is assumed, this model can be solved without factorization approximation for any dynamic correlation function. The solution differs from that obtained from the ideal mode coupling theory (MCT). The latter is equivalent to including only some, positive definite terms in an expression for the memory function. An approximate re-summation of the complete expression suggests that, under the assumption of Gaussian factorization of static fluctuations, mobile particle's motion is always diffusive. In contrast, MCT predicts that the mobile particle becomes localized at a high enough obstacle density. We discuss the implications of these results for models for glassy dynamics.Comment: to be published in Europhys. Let

Tagged particle in a sheared suspension: effective temperature determines density distribution in a slowly varying external potential beyond linear response

We consider a sheared colloidal suspension under the influence of an external potential that varies slowly in space in the plane perpendicular to the flow and acts on one selected (tagged) particle of the suspension. Using a Chapman-Enskog type expansion we derive a steady state equation for the tagged particle density distribution. We show that for potentials varying along one direction only, the tagged particle distribution is the same as the equilibrium distribution with the temperature equal to the effective temperature obtained from the violation of the Einstein relation between the self-diffusion and tagged particle mobility coefficients. We thus prove the usefulness of this effective temperature for the description of the tagged particle behavior beyond the realm of linear response. We illustrate our theoretical predictions with Brownian dynamics computer simulations.Comment: Accepted for publication in Europhys. Let

Microscopic theory for the glass transition in a system without static correlations

We study the orientational dynamics of infinitely thin hard rods of length L, with the centers-of-mass fixed on a simple cubic lattice with lattice constant a.We approximate the influence of the surrounding rods onto dynamics of a pair of rods by introducing an effective rotational diffusion constant D(l),l=L/a. We get D(l) ~ [1-v(l)], where v(l) is given through an integral of a time-dependent torque-torque correlator of an isolated pair of rods. A glass transition occurs at l_c, if v(l_c)=1. We present a variational and a numerically exact evaluation of v(l).Close to l_c the diffusion constant decreases as D(l) ~ (l_c-l)^\gamma, with \gamma=1. Our approach predicts a glass transition in the absence of any static correlations, in contrast to present form of mode coupling theory.Comment: 6 pages, 3 figure

Glass transition in systems without static correlations: a microscopic theory

We present a first step toward a microscopic theory for the glass transition in systems with trivial static correlations. As an example we have chosen N infinitely thin hard rods with length L, fixed with their centers on a periodic lattice with lattice constant a. Starting from the N-rod Smoluchowski equation we derive a coupled set of equations for fluctuations of reduced k-rod densities. We approximate the influence of the surrounding rods onto the dynamics of a pair of rods by introduction of an effective rotational diffusion tensor D and in this way we obtain a self-consistent equation for D. This equation exhibits a feedback mechanism leading to a slowing down of the relaxation. It involves as an input the Laplace transform v_0(l/r) at z=0, l=L/a, of a torque-torque correlator of an isolated pair of rods with distance R=ar. Our equation predicts the existence of a continuous ergodicity-breaking transition at a critical length l_c=L_c/a. To estimate the critical length we perform an approximate analytical calculation of v_0(l/r) based on a variational approach and obtain l_c^{var}=5.68, 4.84 and 3.96 for an sc, bcc and fcc lattice. We also evaluate v_0(l/r) numerically exactly from a two-rod simulation. The latter calculation leads to l_c^{num}=3.45, 2.78 and 2.20 for the corresponding lattices. Close to l_c the rotational diffusion constant decreases as D(l) ~ (l_c - l)^\gamma with \gamma=1 and a diverging time scale t_\epsilon ~ |l_c - l|^{-\delta}, \delta=2, appears. On this time scale the t- and l-dependence of the 1-rod density is determined by a master function depending only on t/t_\epsilon. In contrast to present microscopic theories our approach predicts a glass transition despite the absence of any static correlations.Comment: 22 pages, 7 figures (minor revisions in the text, corrected figures

Stochastic model for the dynamics of interacting Brownian particles

Using the scheme of mesoscopic nonequilibrium thermodynamics, we construct the one- and two- particle Fokker-Planck equations for a system of interacting Brownian particles. By means of these equations we derive the corresponding balance equations. We obtain expressions for the heat flux and the pressure tensor which enable one to describe the kinetic and potential energy interchange of the particles with the heat bath. Through the momentum balance we analyze in particular the diffusion regime to obtain the collective diffusion coefficient in terms of the hydrodynamic and the effective forces acting on the Brownian particles.Comment: latex fil

Mechanical Responses and Stress Fluctuations of a Supercooled Liquid in a Sheared Non-Equilibrium State

A steady shear flow can drive supercooled liquids into a non-equilibrium state. Using molecular dynamics simulations under steady shear flow superimposed with oscillatory shear strain for a probe, non-equilibrium mechanical responses are studied for a model supercooled liquid composed of binary soft spheres. We found that even in the strongly sheared situation, the supercooled liquid exhibits surprisingly isotropic responses to oscillating shear strains applied in three different components of the strain tensor. Based on this isotropic feature, we successfully constructed a simple two-mode Maxwell model that can capture the key features of the storage and loss moduli, even for highly non-equilibrium state. Furthermore, we examined the correlation functions of the shear stress fluctuations, which also exhibit isotropic relaxation behaviors in the sheared non-equilibrium situation. In contrast to the isotropic features, the supercooled liquid additionally demonstrates anisotropies in both its responses and its correlations to the shear stress fluctuations. Using the constitutive equation (a two-mode Maxwell model), we demonstrated that the anisotropic responses are caused by the coupling between the oscillating strain and the driving shear flow. We measured the magnitude of this violation in terms of the effective temperature. It was demonstrated that the effective temperature is notably different between different components, which indicates that a simple scalar mapping, such as the concept of an effective temperature, oversimplifies the true nature of supercooled liquids under shear flow. An understanding of the mechanism of isotropies and anisotropies in the responses and fluctuations will lead to a better appreciation of these violations of the FDT, as well as certain consequent modifications to the concept of an effective temperature.Comment: 15pages, 17figure

Dynamics in Colloidal Liquids near a Crossing of Glass- and Gel-Transition Lines

Within the mode-coupling theory for ideal glass-transitions, the mean-squared displacement and the correlation function for density fluctuations are evaluated for a colloidal liquid of particles interacting with a square-well potential for states near the crossing of the line for transitions to a gel with the line for transitions to a glass. It is demonstrated how the dynamics is ruled by the interplay of the mechanisms of arrest due to hard-core repulsion and due to attraction-induced bond formation as well as by a nearby higher-order glass-transition singularity. Application of the universal relaxation laws for the slow dynamics near glass-transition singularities explains the qualitative features of the calculated time dependence of the mean-squared displacement, which are in accord with the findings obtained in molecular-dynamics simulation studies by Zaccarelli et. al [Phys. Rev. E 66, 041402 (2002)]. Correlation functions found by photon-correlation spectroscopy in a micellar system by Mallamace et. al [Phys. Rev. Lett. 84, 5431 2000)] can be interpreted qualitatively as a crossover from gel to glass dynamics.Comment: 13 pages, 12 figure

Approach to equilibrium for a class of random quantum models of infinite range

We consider random generalizations of a quantum model of infinite range introduced by Emch and Radin. The generalization allows a neat extension from the class $l_1$ of absolutely summable lattice potentials to the optimal class $l_2$ of square summable potentials first considered by Khanin and Sinai and generalised by van Enter and van Hemmen. The approach to equilibrium in the case of a Gaussian distribution is proved to be faster than for a Bernoulli distribution for both short-range and long-range lattice potentials. While exponential decay to equilibrium is excluded in the nonrandom $l_1$ case, it is proved to occur for both short and long range potentials for Gaussian distributions, and for potentials of class $l_2$ in the Bernoulli case. Open problems are discussed.Comment: 10 pages, no figures. This last version, to appear in J. Stat. Phys., corrects some minor errors and includes additional references and comments on the relation to experiment