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Register a new userThree-dimensional imaging of colloidal glasses under steady shear
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Using fast confocal microscopy we image the three-dimensional dynamics of particles in a yielded hard-sphere colloidal glass under steady shear. The structural relaxation, observed in regions with uniform shear, is nearly isotropic but is distinctly different from that of quiescent metastable colloidal fluids. The inverse relaxation time $tau_alpha^{-1}$ and diffusion constant $D$, as functions of the {it local} shear rate $dot{gamma}$, show marked shear thinning with $tau_alpha^{-1} propto D propto dot{gamma}^{0.8}$ over more than two decades in $dot{gamma}$. In contrast, the {it global} rheology of the system displays Herschel-Bulkley behavior. We discuss the possible role of large scale shear localization and other mechanisms in generating this difference.
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We image local structural rearrangements in soft colloidal glasses under small periodic perturbations induced by thermal cycling. Local structural entropy $S_{2}$ positively correlates with observed rearrangements in colloidal glasses. The high $S_{2}$ values of the rearranging clusters in glasses indicate that fragile regions in glasses are structurally less correlated, similar to structural defects in crystalline solids. Slow-evolving high $S_{2}$ spots are capable of predicting local rearrangements long before the relaxations occur, while fluctuation-created high $S_{2}$ spots best correlate with local deformations right before the rearrangement events. Local free volumes are also found to correlate with particle rearrangements at extreme values, although the ability to identify relaxation sites is substantially lower than $S_{2}$. Our experiments provide an efficient structural identifier for the fragile regions in glasses, and highlight the important role of structural correlations in the physics of glasses.
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.
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.
We report experiments on hard sphere colloidal glasses that reveal a type of shear banding hitherto unobserved in soft glasses. We present a scenario that relates this to an instability arising from shear-concentration coupling, a mechanism previously thought unimportant in this class of materials. Below a characteristic shear rate $dotgamma_c$ we observe increasingly non-linear velocity profiles and strongly localized flows. We attribute this trend to very slight concentration gradients (likely to evade direct detection) arising in the unstable flow regime. A simple model accounts for both the observed increase of $dotgamma_c$ with concentration, and the fluctuations observed in the flow.
We perform kinetic Monte Carlo simulations of a distinguishable-particle lattice model of structural glasses with random particle interactions. By varying the interaction distribution and the average particle hopping energy barrier, we obtain an extraordinarily wide range of kinetic fragility. A stretching exponent, characterizing structural relaxation, is found to decrease with the kinetic fragility in agreement with experiments. The most fragile glasses are those exhibiting low hopping barriers and, more importantly, dramatic drops of entropies upon cooling toward the glass transition temperatures. The entropy drops reduce possible kinetic pathways and lead to dramatic slowdowns in the dynamics. In addition, the kinetic fragility is shown to correlate with a thermodynamic fragility.
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