Abstract
Spatially varying electric fields are prevalent throughout nature, such as in nanoporous materials and biological membranes, and technology, e.g, patterned electrodes and van der Waals heterostructures. While uniform fields cause free ions to migrate, for polar fluids they simply reorient the constituent molecules. In contrast, electric field gradients (EFGs) induce a dielectrophoretic force, offering fine control of polar fluids even in the absence of free charges. Despite their vast potential for optimizing fluid behavior, EFGs remain largely unexplored at the microscopic level due to the absence of a rigorous first-principles theory of electrostriction. By integrating state-of-the-art advances in liquid state theory and deep learning, we reveal how EFGs modulate fluid structure and capillarity. We demonstrate 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 manipulate confined fluids-as a powerful mechanism for controlling volumetric capacity in nanopores, holding immense potential for energy storage, selective gas separation, and tunable hysteresis in neuromorphic nanofluidics. Furthermore, by linking nanoscale dielectrocapillarity to macroscopic dielectrowetting, we establish a foundation for field-controlled wetting and adsorption phenomena of polar fluids across length scales.