Hydrodynamic interactions between charged and uncharged Brownian colloids at a fluid-fluid interface.

Hypothesis: The cluster formation and self-assembly of floating colloids at a fluid/fluid interface is a delicate force balance involving deterministic lateral interaction forces, viscous resistance to relative colloid motion along the surface and thermal (Brownian) fluctuations. As the colloid dimensions get smaller, thermal forces and associated drag forces become important and can affect the self assembly into ordered patterns and crystal structures that are the starting point for various materials applications.

Numerics: Langevin dynamic simulations for particle pairs straddling a liquid-liquid interface with a high viscosity contrast are presented to describe the lateral interfacial assembly of particles in Brownian and non-Brownian dominated regimes. These simulations incorporate capillary attraction, electrostatic repulsion, thermal fluctuations and hydrodynamic interactions (HI) between particles (including the effect of the particle immersion depth). Simulation results are presented for neutrally wetted particles which form a contact angle θ=90 at the interface.

Findings: The simulation results suggest that clustering, fractal growth and particle ordering become favorable outcomes at critically large values of the Pe numbers, while smaller Pe numbers exhibit higher probabilities of final configurations where particle motion remains uncorrelated in space and particle pairs are found to be more widely separated especially upon the introduction of HI.