Mechanistic Understanding of the Stochastic Nature of Filamentary Switching in CsFAPbI ₃ Perovskite‐Based Memristors

ABSTRACT Perovskite memristors are redefining the landscape of memory storage and neuromorphic computing by combining rich ion dynamics, ultralow voltage switching, cost‐effective solution processability, and excellent scalability within a single material platform. Harnessing their intrinsic stochasticity in conductive filamentary switching provides a physical route to true random number generation and a unique window into the fundamental physics of resistive switching. Herein, we investigate solution‐processed ITO/Cs 0.1 FA 0.9 PbI 3 /Ag organic–inorganic hybrid halide perovskite (OIHP) memristors that exhibit low voltage switching (∼0.29 V) with distinct cumulative function (∼100x) between ON/OFF states, demonstrating stability of 10 3 cycles and providing a clear mechanism of OIHP‐based memristors, thereby advancing fundamentals of next‐generation neuromorphic computing and practical hurdles in electronics hardware. Investigating the elemental analysis at the buried interface via X‐ray photoelectron spectroscopy (XPS) and energy dispersive X‐ray spectroscopy (EDX) reveal previously overlooked and underexplored phenomena at the ITO‐perovskite junction, offering essential understanding into the switching mechanism. Additionally, pulse stress testing with sharp 500 µs‐wide excitation demonstrates robust endurance and concurrently exposing the intrinsic complexity and dynamic unpredictability of filamentary interactions. These results unveil the mechanistic understanding of FA‐based OIHP memristors and also provide vital insights into their potential in large‐scale, brain‐inspired architectures for neuromorphic computing and secure information processing.