Interstitial Ag+ Engineering Enables Superior Resistive Switching in Quasi-2D Halide Perovskites

Halide perovskite-based memristors are promising neuromorphic devices due to their unique ion migration and interface tunability, yet their conduction mechanisms remain unclear, causing stability and performance issues. Here, we engineer interstitial Ag+ ions within a quasi-two-dimensional (quasi-2D) halide perovskite ((C6H5C2H4NH3)2Csn−1PbnI3n+1) to enhance device stability and controllability. The introduced Ag+ ions occupy organic interlayers, forming thermodynamically stable structures and introducing deep-level energy states without structural distortion, which do not act as non-radiative recombination centers, but instead serve as efficient charge trapping centers that stabilize intermediate resistance states and facilitate controlled filament evolution during resistive switching. This modification also leads to enhanced electron transparency near the Fermi level, contributing to improved charge transport dynamics and device performance. Under external electric fields, these Ag+ ions act as mobile ionic species, facilitating controlled filament formation and stable resistive switching. The resulting devices demonstrate exceptional performance, featuring an ultrahigh on/off ratio (∼108) and low operating voltages (∼0.31 V), surpassing existing benchmarks. Our findings highlight the dual role of Ag+ ions in structural stabilization and conduction modulation, providing a robust approach for high-performance perovskite memristor engineering.