Understanding glass formation is a challenge, because the existence of a true glass state, distinct from liquid and solid, remains elusive: Glasses are liquids that have become too viscous to flow. An old idea, as yet unproven experimentally, is that the dynamics becomes sluggish as the glass transition approaches, because increasingly larger regions of the material have to move simultaneously to allow flow. We introduce new multipoint dynamical susceptibilities to estimate quantitatively the size of these regions and provide direct experimental evidence that the glass formation of molecular liquids and colloidal suspensions is accompanied by growing dynamic correlation length scales.
We use multispeckle dynamic light scattering to measure the dynamic structure factor, , of gels formed by aggregation of colloids. Although the gel is an elastic solid, nearly completely decays on long time scales, with an unusual form, , with and with . A model for restructuring of the gel with aging correctly accounts for this behavior. Aging leads to a dramatic increase in ; however, all data can be scaled on a single master curve, with asymptotically growing linearly with age. This behavior is strikingly similar to that predicted for aging in disordered glassy systems, offering convincing proof of the universality of these concepts.
We use dynamic light scattering and computer simulations to study equilibrium dynamics and dynamic heterogeneity in concentrated suspensions of colloidal hard spheres. Our study covers an unprecedented density range and spans seven decades in structural relaxation time, , including equilibrium measurements above , the location of the glass transition deduced from fitting our data to mode-coupling theory. Instead of falling out of equilibrium, the system remains ergodic above and enters a new dynamical regime where increases with a functional form that was not anticipated by previous experiments, while the amplitude of dynamic heterogeneity grows slower than a power law with , as found in molecular glass formers close to the glass transition.
29 January 2005 in Journal of Physics: Condensed Matter
Measuring, characterizing and modelling the slow dynamics of glassy soft matter is a great challenge, with an impact that ranges from industrial applications to fundamental issues in modern statistical physics, such as the glass transition and the description of out-of-equilibrium systems. Although our understanding of these phenomena is still far from complete, recent simulations and novel theoretical approaches and experimental methods have shed new light on the dynamics of soft glassy materials. In this paper, we review the work of the last few years, with an emphasis on experiments in four distinct and yet related areas: the existence of two different glass states (attractive and repulsive), the dynamics of systems very far from equilibrium, the effect of an external perturbation on glassy materials, and dynamical heterogeneity.
We use conventional and multispeckle dynamic light scattering to investigate the dynamics of a wide variety of jammed soft materials, including colloidal gels, concentrated emulsions, and concentrated surfactant phases. For all systems, the dynamic structure factor f(q,t) exhibits a two-step decay. The initial decay is due to the thermally activated diffusive motion of the scatterers, as indicated by the q−2 dependence of the characteristic relaxation time, where q is the scattering vector. However, due to the constrained motion of the scatterers in jammed systems, the dynamics are arrested and the initial decay terminates in a plateau. Surprisingly, we find that a final, ultraslow decay leads to the complete relaxation of f(q,t), indicative of rearrangements on length scales as large as several microns or tens of microns. Remarkably, for all systems the same very peculiar form is found for the final relaxation of the dynamic structure factor: f(q,t) ∼ exp[−(t/τs)p], with p ≈ 1.5 and τs ∼ q−1, thus suggesting the generality of this behavior. Additionally, for all samples the final relaxation slows down with age, although the aging behavior is found to be sample dependent. We propose that the unusual ultraslow dynamics are due to the relaxation of internal stresses, built into the sample at the jamming transition, and present simple scaling arguments that support this hypothesis.