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Register a new userCluster structure and dynamics in gels and glasses
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The dynamical arrest of gels is the consequence of a well defined structural phase transition, leading to the formation of a spanning cluster of bonded particles. The dynamical glass transition, instead, is not accompanied by any clear structural signature. Nevertheless, both transitions are characterized by the emergence of dynamical heterogeneities. Reviewing recent results from numerical simulations, we discuss the behavior of dynamical heterogeneities in different systems and show that a clear connection with the structure exists in the case of gels. The emerging picture may be also relevant for the more elusive case of glasses. We show, as an example, that the relaxation process of a simple glass-forming model can be related to a reverse percolation transition and discuss further perspective in this direction.
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We study a lattice model of attractive colloids. It is exactly solvable on sparse random graphs. As the pressure and temperature are varied it reproduces many characteristic phenomena of liquids, glasses and colloidal systems such as ideal gel formation, liquid-glass phase coexistence, jamming, or the reentrance of the glass transition.
Following recent X-ray diffraction experiments by Wong, Li, and Safinya on biopolymer gels, we apply Onsager excluded volume theory to a nematic mixture of rigid rods and strong ``$pi/2$ cross-linkers obtaining a long-ranged, highly anisotropic depletion attraction between the linkers. This attraction leads to breakdown of the percolation theory for this class of gels, to breakdown of Onsagers second-order virial method, and to formation of heterogeneities in the form of raft-like ribbons.
We investigate by means of molecular dynamics simulation a coarse-grained polymer glass model focusing on (quasi-static and dynamical) shear-stress fluctuations as a function of temperature T and sampling time $Delta t$. The linear response is characterized using (ensemble-averaged) expectation values of the contributions (time-averaged for each shear plane) to the stress-fluctuation relation $mu_{sf}$ for the shear modulus and the shear-stress relaxation modulus $G(t)$. Using 100 independent configurations we pay attention to the respective standard deviations. While the ensemble-averaged modulus $mu_{sf}(T)$ decreases continuously with increasing T for all $Delta t$ sampled, its standard deviation $delta mu_{sf}(T)$ is non-monotonous with a striking peak at the glass transition. The question of whether the shear modulus is continuous or has a jump-singularity at the glass transition is thus ill-posed. Confirming the effective time-translational invariance of our systems, the $Delta t$-dependence of $mu_{sf}$ and related quantities can be understood using a weighted integral over $G(t)$. This implies that the shear viscosity $eta(T)$ may be readily obtained from the $1/Delta t$-decay of $mu_{sf}$ above the glass transition.
We report measurements of the frequency-dependent shear moduli of aging colloidal systems that evolve from a purely low-viscosity liquid to a predominantly elastic glass or gel. Using microrheology, we measure the local complex shear modulus $G^{*}(omega)$ over a very wide range of frequencies (1 Hz- 100 kHz). The combined use of one- and two-particle microrheology allows us to differentiate between colloidal glasses and gels - the glass is homogenous, whereas the colloidal gel shows a considerable degree of heterogeneity on length scales larger than 0.5 micrometer. Despite this characteristic difference, both systems exhibit similar rheological behavior which evolve in time with aging, showing a crossover from a single power-law frequency dependence of the viscoelastic modulus to a sum of two power laws. The crossover occurs at a time $t_{0}$, which defines a mechanical transition point. We found that the data acquired during the aging of different samples can be collapsed onto a single master curve by scaling the aging time with $t_{0}$. This raises questions about the prior interpretation of two power laws in terms of a superposition of an elastic network embedded in a viscoelastic background. Keywords: Aging, colloidal glass, passive microrheology
We use molecular dynamics computer simulations to investigate the relaxation dynamics of a simple model for a colloidal gel at a low volume fraction. We find that due to the presence of the open spanning network this dynamics shows at low temperature a non-trivial dependence on the wave-vector which is very different from the one observed in dense glass-forming liquids. At high wave vectors the relaxation is due to the fast cooperative motion of the branches of the gel network, whereas at low wave vectors the overall rearrangements of the heterogeneous structure produce the relaxation process.
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