| Summary: | Abstract In the quest to reduce energy consumption, there is a growing demand for technology beyond silicon as electronic materials for neuromorphic artificial intelligence devices. Equipped with the criteria of energy efficiency and excellent adaptability, organohalide perovskites can emulate the characteristics of synaptic functions in the human brain. In this aspect, this study designs and develops CsFAPbI3‐based memristive neuromorphic devices that can switch at low power and show larger endurance by adopting the powder engineering methodology. The neuromorphic characteristics of the CsFAPbI3‐based devices exhibit an ultra‐high paired‐pulse facilitation index for an applied electric stimuli pulse. Moreover, the transition from short‐term to long‐term memory requires ultra‐low energy with long relaxation times. The learning and training cycles illustrate that the CsFAPbI3‐based devices exhibit faster learning and memorization process owing to their larger carrier lifetime compared to other perovskites. The results provide a pathway to attain low‐power neuromorphic devices that are synchronic to the human brain's performance.
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