Electrorotation of leaky-dielectric and conducting microspheres in asymmetric electrolytes and angular velocity reversal

We consider the central problem of polarizable and leaky-dielectric uncharged spherical particle freely suspended in an unbounded nonsymmetric binary electrolyte, which is forced by an ambient time-harmonic uniform electric field. Under the assumption of a “weak field,” we employ the linearized standard electrokinetic model of binary electrolytes to account for such anion/cation asymmetry. A simplified generalized asymmetric dipole-term approximation, valid for a dielectric/conducting microsphere, is analytically derived for an arbitrary Debye scale and for any mismatch between ion diffusivities and valances. A two-peak unified dispersion spectrum covering all range of practical frequencies (KHz to MHz), is found for the case of a rotating electric field (ROT). The angular velocity of a free polarized particle is composed of dielectrophoretic contribution, resulting from the electrical torque (dipole term) as well as from the induced electroosmotic (ICEO) flow field. The two effects usually act in opposite directions. Under ROT excitation, we obtain a cofield rotation at high frequencies (MHz) and a counter-field behavior at low frequencies (KHz). The low-frequency dispersion is generally governed by electric double-layer charging and the high frequency by a Maxwell–Wagner relaxation process. ICEO generally dominates the low-frequency cofield response; however, it can be shown that depending on the electrolyte asymmetry, yet another dielectrophoretic related switching (reversal) point might exist. Furthermore, for large frequencies and depending on the complex permittivity ratio between the particle and electrolyte, we find a second switching point. Explicit expressions for the above two frequency reversal values are obtained in terms of the problem physical parameters and are compared against experimental results. Finally, we provide an analytical solution for the ROT ICEO velocity field of a microsphere as a function of electrolyte asymmetry and Debye length and compare it with numerical simulations.