| In this thesis, three specific research contributions to the use of non-uniform electric field driven colloidal assembly are described. The first relates to experimental work using dielectrophoretic and electrohydrodynamic forces (electroosmosis) to shape three-dimensional colloidal structures. Formation and stabilization of close-packed three-dimensional structures from colloidal silica was demonstrated, using gelation of pluronic F-127 to preserve medium structure against suspension evaporation. Stabilization of ordered structures was shown to be a significant challenge, with many of the conventional techniques for immobilizing colloidal crystals being ineffective. Secondly, the significance of electrohydrodynamic flows resulting from electric and particle concentration (entropic) gradients during the assembly process was demonstrated using numerical simulations based on a thermodynamic framework. These simulations, as well as experimental validation of assembly and the presence of fluid flows, showed that assuming equilibrium behavior (stationary fluid flow), a common assumption for most modelling work to date in these systems, is inappropriate at all but the most dilute concentration cases. Finally, the relevance of multiparticle effects on electric-field induced phase transitions of dielectric colloids was demonstrated. The effect of multiparticle/multiscattering effects on the suspension permittivity were accounted for using semi-empirical continuum permittivity formulations which have been previously shown to describe a wide variety of solid packing structures, including face-centered cubic and other colloidal crystal structures. It was shown that multiparticle effects have a significant impact on both the coexistence (slow phase separation) and spinodal (fast phase separation) behavior of dielectric suspensions, which has not been demonstrated to date using a continuum framework. |
