Specially synthesized silica colloidal spheres with fluorescent cores were used as model electrorheological fluids to experimentally explore structure formation and evolution under conditions of no shear. Using Confocal Scanning Laser Microscopy we measured the location of each colloid in three dimensions. We observed an equilibrium body-centered tetragonal phase and several non-equilibrium structures such as sheet-like labyrinths and isolated chains of colloids. The formation of non-equilibrium structures was studied as a function of the volume fraction, electric field strength and starting configuration of the colloid. We compare our observations to previous experiments, simulations and calculations.

We propose a model that takes into account the effect of flow-modified permittivity (FMP) on electrorheology (ER). Our computer simulation shows that for Mason numbers less than 0.1, ER effects are mainly attributable to the deformation of chain structures, in agreement with earlier theoretical and simulation work. At larger Mason numbers, where chain structures have been destroyed by shear flows, we show that an FMP-induced misalignment between the particle dipole moments and the applied electric field plays a crucial role in producing ER effects. We also identify conditions under which negative ER effects are seen at large Mason numbers.

We propose a model that takes into account the effect of flow-modified permittivity on electrorheology (ER). Due to dielectric relaxation, a shear flow causes the induced particle dipole moments in an ER fluid to tilt in a direction away from the direction of the applied DC electric field. Results from our computer simulation indicate that at high shear rates this misalignment (tilt angle) between the particle dipole moments and the applied electric field plays a crucial role in producing ER effects. By choosing particle-fluid dielectric and conductive mismatches to optimize the tilt angle, our simulation produces ER effects at much higher shear rates than those in earlier simulation work, even though there is no chain structure at these high shear rates. The increase in shear stress due to the applied electric field in our simulation is nearly constant over the wide range of shear rates examined, in qualitative agreement with experimental results. In addition, our model generates results that agree with earlier simulation work at low shear rates, where the particle dipole moments are essetially aligned with the field and the chain model is adequate.

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