We report on a new type of experiment that enables us to monitor spatially and temporally heterogeneous dynamic properties in complex fluids. Our approach is based on the analysis of near-field speckles produced by light diffusely reflected from the superficial volume of a strongly scattering medium. By periodic modulation of an incident speckle beam we obtain pixel-wise ensemble averages of the structure function coefficient, a measure of the dynamic activity. To illustrate the application of our approach we follow the different stages in the drying process of a colloidal thin film. We show that we can access ensemble averaged dynamic properties on length scales as small as ten micrometers over the full field of view.
-- A scientific hurdle in manufacturing solid films by drying colloidal layers is preventing them from fracturing. This paper examines how the drying rate of colloidal liquids influences the particle packing at the nanoscale in correlation with the crack patterns observed at the macroscale. Increasing the drying rate results in more ordered, denser solid structures, and the dried samples have more cracks.Yet, introducing a holding period (at a prescribed point) during the drying protocol results in a more disordered solid structure with significantly less cracks. To interpret these observations, this paper conjectures that a longer drying protocol favors the formation of aggregates. It is further argued that the number and size of the aggregates increase as the drying rate decreases. This results in the formation of a more disordered, porous film from the viewpoint of the particle packing, and a more resistant film, i.e. less cracks, from the macroscale viewpoint.
We have studied the percolation behaviour of deposits for different (2+1)-dimensional models of surface layer formation. The mixed model of deposition was used, where particles were deposited selectively according to the random (RD) and ballistic (BD) deposition rules. In the mixed one-component models with deposition of only conducting particles, the mean height of the percolation layer (measured in monolayers) grows continuously from 0.89832 for the pure RD model to 2.605 for the pure RD model, but the percolation transition belong to the same universality class, as in the 2- dimensional random percolation problem. In two- component models with deposition of conducting and isolating particles, the percolation layer height approaches infinity as concentration of the isolating particles becomes higher than some critical value. The crossover from 2d to 3d percolation was observed with increase of the percolation layer height.
In directionally-dried colloidal dispersions regular bands can appear behind the drying front, inclined at $pm45^circ$ to the drying line. Although these features have been noted to share visual similarities to shear bands in metal, no physical mechanism for their formation has ever been suggested, until very recently. Here, through microscopy of silica and polystyrene dispersions, dried in Hele-Shaw cells, we demonstrate that the bands are indeed associated with local shear strains. We further show how the bands form, that they scale with the thickness of the drying layer, and that they are eliminated by the addition of salt to the drying dispersions. Finally, we reveal the origins of these bands in the compressive forces associated with drying, and show how they affect the optical properties (birefringence) of colloidal films and coatings.
We study how the dynamics of a drying front propagating through a porous medium are affected by small-scale correlations in material properties. For this, we first present drying experiments in micro-fluidic micro-models of porous media. Here, the fluid pressures develop more intermittent dynamics as local correlations are added to the structure of the pore spaces. We also consider this problem numerically, using a model of invasion percolation with trapping, and find that there is a crossover in invasion behaviour associated with the length-scale of the disorder in the system. The critical exponents associated with large enough events are similar to the classic invasion percolation problem, whereas the addition of a finite correlation length significantly affects the exponent values of avalanches and bursts, up to some characteristic size. This implies that the even a weak local structure can interfere with the universality of invasion percolation phenomena.
We study experimentally the origin of heterogeneous dynamics in strongly driven glass-forming systems. Thereto, we apply a well-defined force with a laser line trap on individual colloidal polystyrene probe particles seeded in an emulsion glass composed of droplets of the same size. Fluid and glass states can be probed. We monitor the trajectories of the probe and measure displacements and their distributions. Our experiments reveal intermittent dynamics around a depinning transition at a threshold force. For smaller forces, linear response connects mean displacement and quiescent mean squared displacement. Mode coupling theory calculations rationalize the observations.