Impact of Inverse Squeezing Flow on the Self-Assembly of Oppositely Charged Colloidal Particles under Electric Field

Hydrodynamic interactions (HIs) play a critical role in the self-organization of colloidal suspensions and biological solutions. However, their roles have remained elusive particularly for charged soft matter systems. Here we consider the role of HIs in the self-assembly of oppositely charged colloidal particles, which is a promising candidate for electrical tunable soft materials. We employ the fluid particle dynamics method to consider many-body HIs and the coupling between the colloid, ion, and fluid motions. We find that, under a constant electric field, oppositely charged colloidal particles form clusters and percolate into a gel network, unlike bundlelike aggregates aligned in the field direction observed by Brownian dynamics simulations neglecting HIs. We reveal that the cluster-forming tendency originates from the incompressibility-induced "inverse squeezing flow" effect that dramatically slows down the disaggregation of attached colloids. Our findings indicate that the HI selects a unique kinetic pathway to the nonequilibrium colloidal self-assembly.