The mechanisms of gravity-constrained aggregation in natural colloidal suspensions

Abstract Colloidal settlement in natural aqueous suspensions is effectively compensated by diffusive movement if particles resist aggregation – a state known as colloidal stability. However, if the settling velocity increases upon aggregation, complex structural features emerge from the directional movement induced by gravity. We present a comprehensive modeling study on the evolution of an aggregated three-dimensional structure due to diffusion, surface interactions, and gravity. The systematic investigation of particle geometry and size revealed three mechanisms: (I) aggregation due to spatial confinement of settled particles, (II) aggregation due to differential settling, whereby fast and slow particles collide, (III) inhibition of aggregation due to fractionation of particles with different settling velocity. A 3D visualization tool allowed us to follow the subtle interplay of these mechanisms and the highly dynamic hierarchical self-assembly of aggregates. It revealed how the balance of the different interactions determines the actual rate of aggregation.