Hydrodynamic lubrication in colloidal gels.

Colloidal gels are elasto-plastic materials composed of an out-of-equilibrium, self-assembled network of micron-sized (solid) particles suspended in a fluid. Recent work has shown that far-field hydrodynamic interactions do not change gel structure, only the rate at which the network forms and ages. However, during gel formation, the interplay between short-ranged attractions leading to gelation and equally short-ranged hydrodynamic lubrication interactions remains poorly understood. Here, we therefore study gelation using a range of hydrodynamic descriptions: from single-body (Brownian Dynamics), to pairwise (Rotne-Prager-Yamakawa), to (non-)lubrication-corrected many-body (Stokesian Dynamics). We confirm the current understanding informed by simulations accurate in the far-field. Yet, we find that accounting for lubrication can strongly impact structure at low colloid volume fraction. Counterintuitively, strongly dissipative lubrication interactions also accelerate the aging of a gel, irrespective of colloid volume fraction. Both elements can be explained by lubrication forces facilitating collective dynamics and therefore phase-separation. Our findings indicate that despite the computational cost, lubricated hydrodynamic modeling with many-body far-field interactions is needed to accurately capture the evolution of the gel structure.

Structuring colloidal gels via micro-bubble oscillations.

Locally (re)structuring colloidal gels - micron-sized particles forming a connected network with arrested dynamics - can enable precise tuning of the micromechanical and -rheological properties of the system. A recent experimental study [B. Saint-Michel, G. Petekidis, and V. Garbin, Soft Matter, 2022, 18, 2092] showed that local ordering can be rapidly induced by acoustically modulating an embedded microbubble. Here, we perform Brownian dynamics simulations to understand the mechanical effect of an oscillating microbubble on the next-to-bubble structure of the embedding colloidal gel. Our simulations reveal hexagonal-close-packed structures over a range that is comparable to the amplitude of the oscillations. However, we were unable to reproduce the unexpectedly long-ranged modification of the gel structure - dozens of amplitudes - observed in experiment. This suggests including long-ranged effects, such as fluid flow, should be considered in future computational work.