Dielectrocapillarity for exquisite control of fluids

Abstract: Spatially varying electric fields are prevalent throughout nature and technology, arising from heterogeneity inherent to all physical systems. Inhomogeneous electric fields can originate naturally, such as in nanoporous materials and biological membranes, or be engineered, e.g., with patterned electrodes or layered van der Waals heterostructures. While uniform fields cause free ions to migrate, for polar fluids they simply act to reorient the constituent molecules. In contrast, electric field gradients (EFGs) induce a dielectrophoretic force, offering exquisite electrokinetic control of a fluid, even in the absence of free charge carriers. EFGs, therefore, offer vast potential for optimizing fluid behavior under confinement, such as in nanoporous electrodes, nanofluidic devices, and chemical separation materials. Yet, EFGs remain largely unexplored at the microscopic level owing to the absence of a rigorous, first principles theoretical treatment of electrostrictive effects. By integrating state-of-the-art advances in liquid state theory and deep learning, we reveal how EFGs modulate fluid structure and capillary phenomena. We demonstrate, from first principles, that dielectrophoretic coupling enables tunable control over the liquid-gas phase transition, capillary condensation, and fluid uptake into porous media. Our findings establish "dielectrocapillarity'' -- the use of EFGs to control confined fluids -- as a powerful tool for controlling volumetric capacity in nanopores, which holds immense potential for optimizing energy storage in supercapacitors, selective gas separation, and tunable hysteresis in neuromorphic nanofluidic devices.