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Register a new userIntermittency and non-Gaussian fluctuations in the dynamics of aging colloidal gels
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This paper has been temporarily withdrawn by the authors.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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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
Rigidity percolation (RP) occurs when mechanical stability emerges in disordered networks as constraints or components are added. Here we discuss RP with structural correlations, an effect ignored in classical theories albeit relevant to many liquid-to-amorphous-solid transitions, such as colloidal gelation, which are due to attractive interactions and aggregation. Using a lattice model, we show that structural correlations shift RP to lower volume fractions. Through molecular dynamics simulations, we show that increasing attraction in colloidal gelation increases structural correlation and thus lowers the RP transition, agreeing with experiments. Hence colloidal gelation can be understood as a RP transition, but occurs at volume fractions far below values predicted by the classical RP, due to attractive interactions which induce structural correlation.
The aging behavior of polymer glass, poly(methyl methacrylate), has been investigated through the measurement of ac dielectric susceptibility ata fixed frequency after a temperature shift $Delta T$ ($le $ 20 K)between two temperatures, $T_1$ and $T_2$. A crossover from cumulative aging to non-cumulative aging could be observed with increasing $Delta T$ using a twin temperature ($T$-) shift measurement. Based on a growth law of a dynamical coherent length given by activated dynamics, we obtained a unique coherent length for positive and negative $T$-shifts. The possibility of the existence of temperature chaos in polymer glasses is discussed.
We sandwich a colloidal gel between two parallel plates and induce a radial flow by lifting the upper plate at a constant velocity. Two distinct scenarios result from such a tensile test: ($i$) stable flows during which the gel undergoes a tensile deformation without yielding, and ($ii$) unstable flows characterized by the radial growth of air fingers into the gel. We show that the unstable regime occurs beyond a critical energy input, independent of the gels macroscopic yield stress. This implies a local fluidization of the gel at the tip of the growing fingers and results in the most unstable wavelength of the patterns exhibiting the characteristic scalings of the classical viscous fingering instability. Our work provides a quantitative criterion for the onset of fingering in colloidal gels based on a local shear-induced yielding, in agreement with the delayed failure framework.
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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