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High-bandwidth viscoelastic properties of aging colloidal glasses and gels

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 Publication date 2007
  fields Physics
and research's language is English




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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



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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.
Evolution of the energy landscape during physical aging of glassy materials can be understood from the frequency and strain dependence of the shear modulus but the non-stationary nature of these systems frustrates investigation of their instantaneous underlying properties. Using a series of time dependent measurements we systematically reconstruct the frequency and strain dependence as a function of age for a repulsive colloidal glass undergoing structural arrest. In this manner, we are able to unambiguously observe the structural relaxation time, which increases exponentially with sample age at short times. The yield stress varies logarithmically with time in the arrested state, consistent with recent simulation results, whereas the yield strain is nearly constant in this regime. Strikingly, the frequency dependence at fixed times can be rescaled onto a master curve, implying a simple connection between the aging of the system and the change in the frequency dependent modulus.
We investigate the stress relaxation behavior on the application of step strains to aging aqueous suspensions of the synthetic clay Laponite. The stress exhibits a two-step decay, from which the slow relaxation modes are extracted as functions of the sample ages and applied step strain deformations. Interestingly, the slow time scales that we estimate show a dramatic enhancement with increasing strain amplitudes. We argue that the system ends up exploring the deeper sections of its energy landscape following the application of the step strain.
Motivated by the mean field prediction of a Gardner phase transition between a normal glass and a marginally stable glass, we investigate the off-equilibrium dynamics of three-dimensional polydisperse hard spheres, used as a model for colloidal or granular glasses. Deep inside the glass phase, we find that a sharp crossover pressure $P_{rm G}$ separates two distinct dynamical regimes. For pressure $P < P_{rm G}$, the glass behaves as a normal solid, displaying fast dynamics that quickly equilibrates within the glass free energy basin. For $P>P_{rm G}$, instead, the dynamics becomes strongly anomalous, displaying very large equilibration time scales, aging, and a constantly increasing dynamical susceptibility. The crossover at $P_{rm G}$ is strongly reminiscent of the one observed in three-dimensional spin-glasses in an external field, suggesting that the two systems could be in the same universality class, consistently with theoretical expectations.
97 - H. Bissig , V. Trappe , S. Romer 2003
This paper has been temporarily withdrawn by the authors. We have recently found that noise in the experiments is at the origin of the supposed back-and-forth motion which is discussed in the first version of the paper. As a consequence, figs 4 and 5 as well as their discussion are incorrect. Figure 1 and the general trend of fig. 2 are still valid. At this time, we are uncertain whether or not the short time behavior of cI, shown in fig. 3, is affected by measurement noise. We are working on a new version of the paper, using new techniques that allow us to correct for the experimental noise.
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