Dynamic surfactants for colloidal self-assembly of bilayer superstructures

Colloid-like emulsions and lipid-coated particles contain fluid surfaces where bound macromolecules may laterally diffuse and reorganize. In self-assembling colloidal systems, we hypothesize that surface mobility may impose unique geometric constraints between particles and precisely control their packing in bulk phases. In this work, we use Brownian Dynamics (BD) simulations and analytical theory to understand the self-assembly of colloids coated by surface-mobile polymer brushes. We discover a rich variety of colloidal superstructures with enhanced mechanical properties, including bilayers, crystalline sheets, worm-like aggregates, and gels. Our work may help further the discovery of versatile building blocks and provide extensive design freedom for self-assembly of smart materials.