Colloidal crystallization in the quasi-two-dimensional induced by electrolyte gradients.

We investigated driven crystal formation events in thin layers of sedimented colloidal particles under low salt conditions. Using optical microscopy, we observe particles in a thermodynamically stable colloidal fluid to move radially converging towards cation exchange resin fragments acting as seed particles. When the local particle concentration has become sufficiently large, subsequently crystallization occurs. Brownian dynamics simulations of a 2D system of purely repulsive point-like particles exposed to an attractive potential, yield strikingly similar scenarios, and kinetics of accumulation and micro-structure formation. This offers the possibility of flexibly designing and manufacturing thin colloidal crystals at controlled positions and thus to obtain specific micro-structures not accessible by conventional approaches. We further demonstrate that particle motion is correlated with the existence of a gradient in electrolyte concentration due to the release of electrolyte by the seeds.

Crystalline multilayers of charged colloids in soft confinement: experiment versus theory.

We combine real-space experiments and lattice sum calculations to investigate the phase diagram of charged colloidal particles under soft confinement. In the experiments we explore the equilibrium phase diagram of charged colloidal spheres in aqueous suspensions confined between two parallel charged walls at low background salt concentrations. Motivated by the experiments, we perform lattice sum minimizations to predict the crystalline ground state of point-like Yukawa particles which are exposed to a soft confining wall potential. In the multilayered crystalline regime, we obtain good agreement between the experimental and numerical findings: upon increasing the density we recover the sequence [structure: see text].

Multilayered crystals of macroions under slit confinement.

The crystalline ground state of macroions confined between two neutral parallel plates in the presence of their homogeneously spread counterions is calculated by lattice sum minimization of candidate phases involving up to six layers. For increasing macroion density, a cascade of solid-solid transitions is found involving various multilayered crystals. The cascade includes triangular monolayer and buckled bilayer as well as rhombic, squared and triangular phase structures.