Spinodal decomposition in a model colloid-polymer mixture in microgravity.

We study phase separation in a deeply quenched colloid-polymer mixture in microgravity on the International Space Station using small-angle light scattering and direct imaging. We observe a clear crossover from early-stage spinodal decomposition to late-stage, interfacial-tension-driven coarsening. Data acquired over 5 orders of magnitude in time show more than 3 orders of magnitude increase in domain size, following nearly the same evolution as that in binary liquid mixtures. The late-stage growth approaches the expected linear growth rate quite slowly.

Time-dependent strength of colloidal gels.

Colloidal silica gels are shown to stiffen with time, as demonstrated by both dynamic light scattering and bulk rheological measurements. Their elastic moduli increase as a power law with time, independent of particle volume fraction; however, static light scattering indicates that there are no large-scale structural changes. We propose that increases in local elasticity arising from bonding between neighboring colloidal particles can account for the strengthening of the network, while preserving network structure.

Limits to gelation in colloidal aggregation.

We show that the dynamics of large fractal colloid aggregates are well described by a combination of translational and rotational diffusion and internal elastic fluctuations, allowing both the aggregate size and internal elasticity to be determined by dynamic light scattering. The comparison of results obtained in microgravity and on Earth demonstrates that cluster growth is limited by gravity-induced restructuring. In the absence of gravity, thermal fluctuations ultimately inhibit fractal growth and set the fundamental limitation to the lowest volume fraction which will gel.

Rideal lecture. Universal features of the fluid to solid transition for attractive colloidal particles.

Attractive colloidal particles can exhibit a fluid to solid phase transition if the magnitude of the attractive interaction is sufficiently large, if the volume fraction is sufficiently high, and if the applied stress is sufficiently small. The nature of this fluid to solid transition is similar for many different colloid systems, and for many different forms of interaction. The jamming phase transition captures the common features of these fluid to solid translations, by unifying the behavior as a function of the particle volume fraction, the energy of interparticle attractions, and the applied stress. This paper describes the applicability of the jamming state diagram, and highlights those regions where the fluid to solid transition is still poorly understood. It also presents new data for gelation of colloidal particles with an attractive depletion interaction, providing more insight into the origin of the fluid to solid transition.

Origin of stability in sedimentation.

Velocity fluctuations and particle concentrations are studied in a liquid fluidized bed to investigate the origin of steady state sedimentation. Both the velocity fluctuations and the particle concentrations are found to strongly depend on height. A flux balance model shows why the bed is stable: velocity fluctuations drive a downward particle flux that is compensated by an upward particle flux stemming from an excess flow velocity due to the stratification in concentration. Our results show that in steady state the magnitudes of the fluctuations are related to the degree of stratification.

Nonuniversal velocity fluctuations of sedimenting particles.

Velocity fluctuations in sedimentation are studied to investigate the origin of a hypothesized universal scale [P. N. Segre, E. Herbolzheimer, and P. M. Chaikin, Phys. Rev. Lett. 79, 2574 (1997)]. Our experiments show that fluctuations decay continuously in time for sufficiently thick cells, never reaching steady state. Simulations and scaling arguments suggest that the decay arises from increasing vertical stratification of particle concentration due to spreading of the sediment front. The results suggest that the velocity fluctuations in sedimentation depend sensitively on cell geometry.

Jamming phase diagram for attractive particles.

A wide variety of systems, including granular media, colloidal suspensions and molecular systems, exhibit non-equilibrium transitions from a fluid-like to a solid-like state, characterized solely by the sudden arrest of their dynamics. Crowding or jamming of the constituent particles traps them kinetically, precluding further exploration of the phase space. The disordered fluid-like structure remains essentially unchanged at the transition. The jammed solid can be refluidized by thermalization, through temperature or vibration, or by an applied stress. The generality of the jamming transition led to the proposal of a unifying description, based on a jamming phase diagram. It was further postulated that attractive interactions might have the same effect in jamming the system as a confining pressure, and thus could be incorporated into the generalized description. Here we study experimentally the fluid-to-solid transition of weakly attractive colloidal particles, which undergo markedly similar gelation behaviour with increasing concentration and decreasing thermalization or stress. Our results support the concept of a jamming phase diagram for attractive colloidal particles, providing a unifying link between the glass transition, gelation and aggregation.

Glasslike kinetic arrest at the colloidal-gelation transition.

We show that gelation of weakly attractive colloids is remarkably similar to the colloidal glass transition. Like the glass transition, dynamic light scattering functions near gelation scale with scattering vector, and exhibits a two-step decay with a power-law divergence of the final decay time. Like the glass transition, static light scattering does not change upon gelation. These results suggest that, like the glass transition, gelation results from kinetic arrest due to crowding of clusters, and that both gelation and the glass transition are manifestations of a more general jamming transition.

An effective gravitational temperature for sedimentation.

The slow sedimentation of suspensions of solid particles in a fluid results in complex phenomena that are poorly understood. For a low volume fraction (phi) of particles, long-range hydrodynamic interactions result in surprising spatial correlations in the velocity fluctuations; these are reminiscent of turbulence, even though the Reynolds number is very low. At higher values of phi, the behaviour of sedimentation remains unclear; the upward back-flow of fluid becomes increasingly important, while collisions and crowding further complicate inter-particle interactions. Concepts from equilibrium statistical mechanics could in principle be used to describe the fluctuations and thereby provide a unified picture of sedimentation, but one essential ingredient--an effective temperature that provides a mechanism for thermalization--is missing. Here we show that the gravitational energy of fluctuations in particle number can act as an effective temperature. Moreover, we demonstrate that the high-phi behaviour is in fact identical to that at low phi, provided that the suspension viscosity and sedimentation velocity are scaled appropriately, and that the effects of particle packing are included.