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Ion concentration polarization (CP, current-induced concentration gradientadjacent to a charge-selective interface) has been well studied forsingle-phase mixed conductors (e.g., liquid electrolyte), but multiphase CP hasbeen rarely addressed in literature. In our recent publication, we proposedthat CP above certain threshold currents can flip the phase distribution inmultiphase ion-intercalation nanofilms sandwiched by ion-blocking electrodes.We call this phenomenon as multiphase polarization (MP). We then proposed thatMP can further lead to nonvolatile interfacial resistive switching (RS) forasymmetric electrodes with ion-modulated electron transfer, which theory canreproduce the experimental results of LTO memristors. In this work, we derive acomprehensive 2D phase-field model for coupled ion-electron transport inion-intercalation materials, with surface effects including electron transferkinetics, non-neutral wetting, energy relaxation, and surface charge. Then weuse the model to study MP. We present time evolution of phase boundaries, andanalyze the switching time, current, energy, and cyclic voltammetry, forvarious boundary conditions. We find that the switching performance can beimproved significantly by manipulating surface conditions and meanconcentration. Finally, we discuss the prospects of MP-based memories andpossible extensions of the current model.

Multiphase polarization in ion-intercalation nanofilms: general theory including various surface effects and memory applications