Compositional Engineering of Monocrystalline Metal Halide Perovskite Memristors for Multistate Non‐Volatile Operation

Abstract Metal halide perovskite (MHP) memristors hold great promise for next‐generation memory and neuromorphic computing. However, challenges such as stability and endurance hinder both their performance and a deeper understanding of their working mechanisms. Advances in thin monocrystalline MHP memristors have demonstrated improved endurance due to the absence of grain boundaries, which makes them an ideal platform for systematically identifying key factors influencing device performance. Thus, evaluating the compositional effects on monocrystalline MHP memristors within a consistent device architecture serves as a powerful approach to deepen understanding of the system and guide the development of application‐oriented devices. This strategy is used to fabricate the first memristor based on a mixed‐halide thin perovskite monocrystal, which enables multistate non‐volatile memristive operation. Furthermore, precise compositional engineering allows control over defect density, which affects the materials’ ionic properties and determines key device performance parameters. This study unlocks multistate properties in non‐volatile memristors and provides critical insights into defect density effects, paving the way for high‐density storage in neuromorphic computing.