Dipolar solvent contributions for transient nanoscale electroosmotic flow

Abstract

Electrohydrodynamic flows of electrolytes with low to moderate ion concentration at the nanoscale are significantly influenced by the molecular structure of water-like polar solvents within the electric double layer (EDL). Moreover, unlike in microfluidics, at these length scales the time scale of evolution of EDL often becomes comparable to the consequent fluidic phenomena of interest. While continuum descriptions to model such phenomena typically assume a constant dielectric and viscous solvent background, this study incorporates dipolar solvent physics. Specifically, both dielectric saturation and the viscoelectric effect are implemented together into a Poisson-Nernst-Planck-Stokes framework, using the Langevin-Bikerman solvent permittivity distribution and empirical viscoelectric coefficients, respectively. Numerical simulations in a one-dimensional geometry reveal substantial modifications to the electrohydrodynamic body force density and transient electroosmotic mobility during EDL evolution. The magnitude and temporal evolution of these corrections are characterized across parametric regimes, revealing systematic departures from standard constant-permittivity and constant-viscosity models, with electroosmotic mobility reductions of up to 65% governed by a characteristic dimensionless parameter. The results predict a characteristic frequency-dependent transition in electroosmotic mobility and dipolar solvent corrections in emerging MHz AC electrokinetic flows. The results provide a solvent-consistent continuum framework for transient nanoscale electroosmotic flows and quantify the impact of molecular solvent structure on electrohydrodynamic transport relevant to modern nanofluidic applications.

16 pages, 8 figures