arXiv subjects

Grzegorz Szamel

Publications and source records attributed to Grzegorz Szamel.

At least 91 records · Page 5Linked to original sources

arXiv2009

Diverging length scale of the inhomogeneous mode-coupling theory: a numerical investigation

Biroli et al.'s extension of the standard mode-coupling theory to inhomogeneous equilibrium states [Phys. Rev. Lett. 97, 195701 (2006)] allowed them to identify a characteristic length scale that diverges upon approaching the mode-coupling transition. We present a numerical investigation of this length scale. To this end we derive and numerically solve equations of motion for coefficients in the small q expansion of the dynamic susceptibility $χ_{\mathbf{q}}(\mathbf{k};t)$ that describes the change of the system's dynamics due to an external inhomogeneous potential. We study the dependence of the characteristic length scale on time, wave-vector, and on the distance from the mode-coupling transition. We verify scaling predictions of Biroli et al. In addition, we find that the numerical value of the diverging length scale qualitatively agrees with lengths obtained from four-point correlation functions. We show that the diverging length scale has very weak k dependence, which contrasts with very strong $k$ dependence of the $q\to 0$ limit of the susceptibility, $χ_{\mathbf{q}=0}(\mathbf{k};t)$. Finally, we compare the diverging length obtained from the small q expansion to that resulting from an isotropic approximation applied to the equation of motion for the dynamic susceptibility $χ_{\mathbf{q}}(\mathbf{k};t)$.

cond-mat.stat-mech↗

arXiv2009

Anisotropic spatially heterogeneous dynamics on the $α$ and $β$ relaxation time scales studied via a four-point correlation function

We examine the anisotropy of a four-point correlation function $G_4(\vec{k},\vec{r};t)$ and it's associated structure factor $S_4(\vec{k},\vec{q};t)$ calculated using Brownian Dynamics computer simulations of a model glass forming system. These correlation functions measure the spatial correlations of the relaxation of different particles, and we examine the time and temperature dependence of the anisotropy. We find that the anisotropy is strongest at nearest neighbor distances at time scales corresponding to the peak of the non-Gaussian parameter $α_2(t) = 3 < δr^4(t) >/[ 5 < δr^2(t) >^2] - 1$, but is still pronounced around the $α$ relaxation time. We find that the structure factor $S_4(\vec{k},\vec{q};t)$ is anisotropic even for the smallest wave vector accessible in our simulation suggesting that our system (and other systems commonly used in computer simulations) may be too small to extract the $\vec{q} \to 0$ limit of the structure factor. We find that the determination of a dynamic correlation length from $S_4(\vec{k},\vec{q};t)$ is influenced by the anisotropy. We extract an effective anisotropic dynamic correlation length from the small $q$ behavior of $S_4(\vec{k},\vec{q};t)$.

cond-mat.soft↗

arXiv2008

Three-point susceptibilities $χ_n(k;t)$ and $χ_n^s(k;t)$: mode-coupling approximation

Recently, it was argued that a three-point susceptibility equal to the density derivative of the intermediate scattering function, $χ_n(k;t) = d F(k;t)/d n$, enters into an expression for the divergent part of an integrated four-point dynamic density correlation function of a colloidal suspension [Berthier \textit{et al.}, J. Chem. Phys. \textbf{126}, 184503 (2007)]. We show that, within the mode-coupling theory, the equation of motion for $χ_n(k;t)$ is essentially identical as the equation of motion for the $\mathbf{q}\to 0$ limit of the three-point susceptibility $χ_{\mathbf{q}}(\mathbf{k};t)$ introduced by Biroli \textit{et al.} [Phys. Rev. Lett. \textbf{97}, 195701 (2006)]. We present a numerical solution of the equation of motion for $χ_n(k;t)$. We also derive and numerically solve an equation of motion for the density derivative of the self-intermediate scattering function, $χ_n^s(k;t) = d F^s(k;t)/d n$. We contrast the wave vector dependence of $χ_n(k;t)$ and $χ_n^s(k;t)$.

cond-mat.soft↗

arXiv2008

Divergent four-point dynamic density correlation function of a glassy colloidal suspension: a diagrammatic approach

We use a recently derived diagrammatic formulation of the dynamics of interacting Brownian particles [G. Szamel, J. Chem. Phys. 127, 084515 (2007)] to study a four-point dynamic density correlation function. We re-sum a class of diagrams which separate into two disconnected components upon cutting a single propagator. The resulting formula for the four-point correlation function can be expressed in terms of three-point functions closely related to the three-point susceptibility introduced by Biroli et al. [Phys. Rev. Lett. 97, 195701 (2006)] and the standard two-point correlation function. The four-point function has a structure very similar to that proposed by Berthier and collaborators [Science 310, 1797 (2005), J. Chem. Phys. 126, 184503 (2007)]. It exhibits a small wave vector divergence at the mode-coupling transition.

cond-mat.stat-mech↗

arXiv2007

Dynamics of interacting Brownian particles: a diagrammatic formulation

We present a diagrammatic formulation of a theory for the time dependence of density fluctuations in equilibrium systems of interacting Brownian particles. To facilitate derivation of the diagrammatic expansion we introduce a basis that consists of orthogonalized many-particle density fluctuations. We obtain an exact hierarchy of equations of motion for time-dependent correlations of orthogonalized density fluctuations. To simplify this hierarchy we neglect contributions to the vertices from higher-order cluster expansion terms. An iterative solution of the resulting equations can be represented by diagrams with three and four-leg vertices. We analyze the structure of the diagrammatic series for the time-dependent density correlation function and obtain a diagrammatic interpretation of reducible and irreducible memory functions. The one-loop self-consistent approximation for the latter function coincides with mode-coupling approximation for Brownian systems that was derived previously using a projection operator approach.

cond-mat.soft↗

arXiv2006

Anisotropic spatially heterogeneous dynamics in a model glass-forming binary mixture

We calculated a four-point correlation function G_4(k,r;t) and the corresponding structure factor S_4(k,q;t) for a model glass-forming binary mixture. These functions measure the spatial correlations of the relaxation of different particles. We found that these four-point functions are anisotropic and depend on the angle between vectors k and r (or q). The anisotropy is the strongest for times somewhat longer than the beta relaxation time but it is quite pronounced even for times comparable to the alpha relaxation time, tau_alpha. At the lowest temperatures S_4(k,q;tau_alpha) is strongly anisotropic even for the smallest wavevector q accessible in our simulation.

cond-mat.stat-mech↗

arXiv2006

Four-point susceptibility of a glass-forming binary mixture: Brownian dynamics

We study the four-point dynamic susceptibility $χ_4(t)$ obtained from Brownian dynamics computer simulations of the Kob-Andersen Lennard-Jones mixture. We compare the results of the simulations with qualitative predictions of the mode-coupling theory. In addition, we test an estimate of the four-point susceptibility recently proposed by Berthier \textit{et al.} [Science, \textbf{310}, 1797 (2005)].

cond-mat.soft↗

arXiv2005

Efficient Monte Carlo simulation of a glass forming binary mixture

We propose and use a novel, hybrid Monte Carlo algorithm that combines configurational bias particle swaps with parallel tempering. We use this new method to simulate a standard model of a glass forming binary mixture above and below the so-called mode-coupling temperature, Tmct. We find that an ansatz that was used previously to extrapolate thermodynamic quantities to temperatures below Tmct breaks down in the vicinity of the mode-coupling temperature. Thus, previous estimates of the so-called Kauzmann temperature need to be reexamined. Also, we find that the Adam-Gibbs relations D ~ exp(-a/TSc) and tau ~ exp(b/TSc), which connect the diffusion coefficient D and the relaxation time tau with the configurational entropy Sc, are valid for all temperatures for which the configurational and vibrational contributions to the free energy decouple.

cond-mat.soft↗

arXiv2005

Nature of the Breakdown in the Stokes-Einstein Relationship in a Hard Sphere Fluid

Molecular Dynamics simulations of high density hard sphere fluids clearly show a breakdown of the Stokes-Einstein equation (SE). This result has been conjectured to be due to the presence of mobile particles, i.e., ones which have the propensity to "hop" distances which are integer multiples of the interparticle distance. We conclusively show that, even though the whole liquid violates the SE equation at high densities, the sedentary particles, i.e., ones complementary to the "hoppers", obey the SE relationship. These results strongly support the notion that the unusual dynamics of fluids near vitrification are caused exclusively by the presence of hopping particles.

cond-mat.mtrl-sci↗

arXiv2005

Relaxation in a glassy binary mixture: Comparison of the mode-coupling theory to a Brownian dynamics simulation

We solved the mode-coupling equations for the Kob-Andersen binary mixture using the structure factors calculated from Brownian dynamics simulations of the same system. We found, as was previously observed, that the mode-coupling temperature, Tc, inferred from simulations is about two times greater than that predicted by the theory. However, we find that many time dependent quantities agree reasonably well with the predictions of the mode-coupling theory if they are compared at the same reduced temperature epsilon = (T-Tc)/Tc, and if epsilon is not too small. Specifically, the simulation results for the incoherent intermediate scattering function, the mean square displacement, the relaxation time and the self-diffusion coefficient agree reasonably well with the predictions of the mode-coupling theory. We find that there are substantial differences for the non-Gaussian parameter. At small reduced temperatures the probabilities of the logarithm of single particle displacements demonstrate that there is hopping-like motion present in the simulations, and this motion is not predicted by the mode-coupling theory. The wave vector dependent relaxation time is shown to be qualitatively different than the predictions of the mode-coupling theory for temperatures where hopping-like motion is present.

cond-mat.soft↗

arXiv2005

Time scale for the onset of Fickian diffusion in supercooled liquids

We propose a quantitative measure of a time scale on which Fickian diffusion sets in for supercooled liquids and use Brownian Dynamics computer simulations to determine the temperature dependence of this onset time in a Lennard-Jones binary mixture. The time for the onset of Fickian diffusion ranges between 6.5 and 31 times the $α$ relaxation time (the $α$ relaxation time is the characteristic relaxation time of the incoherent intermediate scattering function). The onset time increases faster with decreasing temperature than the $α$ relaxation time. Mean squared displacement at the onset time increases with decreasing temperature.

cond-mat.dis-nn↗

arXiv2005

Relaxation in a glassy binary mixture: Mode-coupling-like power laws, dynamic heterogeneity and a new non-Gaussian parameter

We examine the relaxation of the Kob-Andersen Lennard-Jones binary mixture using Brownian dynamics computer simulations. We find that in accordance with mode-coupling theory the self-diffusion coefficient and the relaxation time show power-law dependence on temperature. However, different mode-coupling temperatures and power laws can be obtained from the simulation data depending on the range of temperatures chosen for the power-law fits. The temperature that is commonly reported as this system's mode-coupling transition temperature, in addition to being obtained from a power law fit, is a crossover temperature at which there is a change in the dynamics from the high temperature homogeneous, diffusive relaxation to a heterogeneous, hopping-like motion. The hopping-like motion is evident in the probability distributions of the logarithm of single-particle displacements: approaching the commonly reported mode-coupling temperature these distributions start exhibiting two peaks. Notably, the temperature at which the hopping-like motion appears for the smaller particles is slightly higher than that at which the hopping-like motion appears for the larger ones. We define and calculate a new non-Gaussian parameter whose maximum occurs approximately at the time at which the two peaks in the probability distribution of the logarithm of displacements are most evident.

cond-mat.soft↗

arXiv2004

Lifetime of dynamic heterogeneities in a binary Lennard-Jones mixture

A four-time correlation function was calculated using a computer simulation of a binary Lennard-Jones mixture. The information content of the four-time correlation function is similar to that of four-time correlation functions measured in NMR experiments. The correlation function selects a sub-ensemble and analyzes its dynamics after some waiting time. The lifetime of the sub-ensemble selected by the four-time correlation function is calculated, and compared to the lifetimes of slow sub-ensembles selected using two different definitions of mobility, and to the $α$ relaxation time.

cond-mat.soft↗

arXiv2004

Is a "homogeneous" description of dynamic heterogeneities possible?

We study the simplest model of dynamic heterogeneities in glass forming liquids: one-spin facilitated kinetic Ising model introduced by Fredrickson and Andersen [G.H. Fredrickson and H.C. Andersen, Phys. Rev. Lett. 53, 1244 (1984); J. Chem. Phys. 83, 5822 (1985)]. We show that the low-temperature, long-time behavior of the density autocorrelation function predicted by a scaling approach can be obtained from a self-consistent mode-coupling-like approximation.

cond-mat.stat-mech↗

arXiv2004

Independence of the relaxation of a supercooled fluid of its microscopic dynamics: need for yet another extension of the mode-coupling theory

Using Brownian Dynamics computer simulations we show that the relaxation of a supercooled Brownian system is qualitatively the same as that of a Newtonian system. In particular, near the so-called mode-coupling transition temperature, dynamic properties of the Brownian system exhibit the same deviations from power-law behavior as those of the Newtonian one. Thus, similar dynamical events cut off the idealized mode-coupling transition in Brownian and Newtonian systems. We discuss implications of this finding for extended mode-coupling theory. In addition, we point out and discuss the difference between our findings and experimental results, and present an alternative interpretation of some of our simulation data.

cond-mat.soft↗

arXiv2004

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.

cond-mat.soft↗

arXiv2004

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.

cond-mat.soft↗

arXiv2003

Colloidal glass transition: Beyond mode-coupling theory

A new theory for dynamics of concentrated colloidal suspensions and the colloidal glass transition is proposed. The starting point is the memory function representation of the density correlation function. The memory function can be expressed in terms of a time-dependent pair-density correlation function. An exact, formal equation of motion for this function is derived and a factorization approximation is applied to its evolution operator. In this way a closed set of equations for the density correlation function and the memory function is obtained. The theory predicts an ergodicity breaking transition similar to that predicted by the mode-coupling theory, but at a higher density.

cond-mat.soft↗