Unraveling Conductive Filament Formation in High Performance Halide Perovskite Memristor

Halide perovskites (HPs) are promising materials for memristor devices because of their unique characteristics. In this study, nonvolatile resistive switching memory devices based on thick MAPbI₃ perovskite (800 nm) films with structure FTO/MAPbI₃/polymethyl methacrylate (PMMA)/Ag are presented. Reproducible and reliable bipolar switching characteristics are demonstrated with an ultra-low operating voltage (−0.1 V), high ON/OFF ratio (10⁶), endurance (>2 × 10³ times) and a record retention time (>10⁵ s). The I–V curve of the first cycle exhibits self-formed conductive filaments. These are attributed to the presence of metallic Pb resulting from an excess of PbI₂ in the perovskite film. The subsequent activation process involves the formation of conductive filaments, consisting of either iodide vacancies or migrated charged metals. Numerical simulations are then carried out to understand the nature of these conductive filaments and the role of the internal electric field in the migration of iodide ions, iodide vacancies, and Ag cations. Finally, an exhaustive model is proposed that explains the set and reset processes governing the first voltage cycle and the steady state, at different voltage ranges. In summary, this work offers a novel and thorough perspective of the complete resistive switching (RS) behavior in a MAPbI₃/buffer/Ag memristor, supported by numerical simulations.