Direct imaging elucidates ionic memory in two-dimensional nanochannels

Abstract

Abstract Nanofluidic memristors promise brain-inspired information processing with ions, yet their microscopic origin remains debated. So far, ionic memory has been attributed to ion-specific interactions, dynamic wetting, chemical reactions or mechanical deformations, yet typically without direct experimental evidence. Here, by combining operando interferometric imaging with electrokinetic measurements, we directly visualize voltage-induced blistering of the confining walls of two-dimensional (2D) nanochannels as the key origin of memristive hysteresis. We identify two distinct classes of blisters: unidirectional, driven by electrostatic forces on surface charges, and bidirectional, arising from osmotic pressure due to concentration polarization. This mechanistic framework explains device evolution and device-to-device variability, and reframes stochastic blistering as a functional design element. Our results constitute a direct proof of electromechanical coupling as a robust pathway to ionic memory in 2D nanochannels and open routes towards high-performance ionic memristors and electrically actuated nanofluidic valves.