Molecular dynamics simulations of the Johari-Goldstein relaxation in a molecular liquid

Molecular dynamics simulations (mds) were carried out to investigate the reorientational motion of a rigid (fixed bond length), asymmetric diatomic molecule in the liquid and glassy states. In the latter the molecule reorients via large-angle jumps, which we identify with the Johari-Goldstein (JG) dynamics. This relaxation process has a broad distribution of relaxation times, and at least deeply in the glass state, the mobility of a given molecule remains fixed over time; that is, there is no dynamic exchange among molecules. Interestingly, the JG relaxation time for a molecule does not depend on the local density, although the non-ergodicity factor is weakly correlated with the packing efficiency of neighboring molecules. In the liquid state the frequency of the JG process increases significantly, eventually subsuming the slower alpha-relaxation. This evolution of the JG-motion into structural relaxation underlies the correlation of many properties of the JG- and alpha-dynamics.Comment: 12 pages, 6 figure

Origin of the slow dynamics and the aging of a soft glass

We study by light microscopy a soft glass consisting of a compact arrangement of polydisperse elastic spheres. We show that its slow and non-stationary dynamics results from the unavoidable small fluctuations of temperature, which induce intermittent local mechanical shear in the sample, because of thermal expansion and contraction. Temperature-induced shear provokes both reversible and irreversible rearrangements whose amplitude decreases with time, leading to an exponential slowing down of the dynamics with sample age.Comment: published in PRL 97, 238301, 200

Equilibrium and non-equilibrium fluctuations in a glass-forming liquid

Glass-forming liquids display strong fluctuations -- dynamical heterogeneities -- near their glass transition. By numerically simulating a binary Weeks-Chandler-Andersen liquid and varying both temperature and timescale, we investigate the probability distributions of two kinds of local fluctuations in the non-equilibrium (aging) regime and in the equilibrium regime; and find them to be very similar in the two regimes and across temperatures. We also observe that, when appropriately rescaled, the integrated dynamic susceptibility is very weakly dependent on temperature and very similar in both regimes.Comment: v1: 5 pages, 4 figures v2: 5 pages, 4 figures. Now includes results at three temperatures, two of them above T_{MCT} and one below T_{MCT}; and more extensive discussion of connections to experiment

Binary mixture of hard disks as a model glass former: Caging and uncaging

I have proposed a measure for the cage effect in glass forming systems. A binary mixture of hard disks is numerically studied as a model glass former. A network is constructed on the basis of the colliding pairs of disks. A rigidity matrix is formed from the isostatic (rigid) sub--network, corresponding to a cage. The determinant of the matrix changes its sign when an uncaging event occurs. Time evolution of the number of the uncaging events is determined numerically. I have found that there is a gap in the uncaging timescales between the cages involving different numbers of disks. Caging of one disk by two neighboring disks sustains for a longer time as compared with other cages involving more than one disk. This gap causes two--step relaxation of this system

On the static length of relaxation and the origin of dynamic heterogeneity in fragile glass-forming liquids

The most puzzling aspect of the glass transition observed in laboratory is an apparent decoupling of dynamics from structure. In this paper we recount the implication of various theories of glass transition for the static correlation length in an attempt to reconcile the dynamic and static lengths associate with the glass problem. We argue that a more recent characterization of the static relaxation length based on the bond ordering scenario, as the typical length over which the energy fluctuations are correlated, is more consistent with, and indeed in perfect agreement with the typical linear size of the dynamically heterogeneous domains observed in deeply supercooled liquids. The correlated relaxation of bonds in terms of energy is therefore identified as the physical origin of the observed dynamic heterogeneity.Comment: 6 pages, 1 figur

1/d1/d Expansion for kk-Core Percolation

The physics of $k$-core percolation pertains to those systems whose constituents require a minimum number of $k$ connections to each other in order to participate in any clustering phenomenon. Examples of such a phenomenon range from orientational ordering in solid ortho-para ${\rm H}_2$ mixtures to the onset of rigidity in bar-joint networks to dynamical arrest in glass-forming liquids. Unlike ordinary ($k=1$) and biconnected ($k=2$) percolation, the mean field $k\ge3$-core percolation transition is both continuous and discontinuous, i.e. there is a jump in the order parameter accompanied with a diverging length scale. To determine whether or not this hybrid transition survives in finite dimensions, we present a $1/d$ expansion for $k$-core percolation on the $d$-dimensional hypercubic lattice. We show that to order $1/d^3$ the singularity in the order parameter and in the susceptibility occur at the same value of the occupation probability. This result suggests that the unusual hybrid nature of the mean field $k$-core transition survives in high dimensions.Comment: 47 pages, 26 figures, revtex

Investigation of qq-dependent dynamical heterogeneity in a colloidal gel by x-ray photon correlation spectroscopy

We use time-resolved X-Photon Correlation Spectroscopy to investigate the slow dynamics of colloidal gels made of moderately attractive carbon black particles. We show that the slow dynamics is temporally heterogeneous and quantify its fluctuations by measuring the variance $\chi$ of the instantaneous intensity correlation function. The amplitude of dynamical fluctuations has a non-monotonic dependence on scattering vector $q$, in stark contrast with recent experiments on strongly attractive colloidal gels [Duri and Cipelletti, \textit{Europhys. Lett.} \textbf{76}, 972 (2006)]. We propose a simple scaling argument for the $q$-dependence of fluctuations in glassy systems that rationalizes these findings.Comment: Final version published in PR