Embedding Horizontally‐Aligned MAPbI 3 Perovskite Nanowires into TIPS‐Pentacene Films Enables High‐Performance Optoelectronic Synaptic Transistors

ABSTRACT Optoelectronic synapses integrate light detection and data‐processing in a single device, emerging as pivotal building blocks for efficient neuromorphic computing. The development of high‐performance optoelectronic synapses hinges on the discovery and engineering of advanced functional materials. This work presents a high‐performance optoelectronic synaptic transistor based on a MAPbI 3 /TIPS‐pentacene heterostructure, where horizontally aligned MAPbI 3 nanowires are grown via nanogroove‐confined recrystallization and conformally encapsulated by a spin‐coated TIPS‐pentacene layer. This rational design leverages full‐visible‐spectrum absorption and a type‐II heterointerface to achieve efficient charge separation and prolonged charge retention time. The resulting heterostructure device exhibits superior optoelectronic performance over single‐component TIPS devices, and emulates core synaptic functionalities, including enhanced excitatory postsynaptic currents tunable via optical spike parameters, a paired‐pulse facilitation index with over 200% enhancement across broad visible wavelengths and time intervals, and improved linear long‐term potentiation/depression with a two‐fold expanded maximum‐to‐minimum conductance ratio ( G max / G min ) of 19. When deployed in neuromorphic computing simulations, the heterojunction device achieves 96% accuracy in MNIST handwritten digit recognition and enables reliable decoding of International Morse code for optical communication. This work verifies that solution‐processed perovskite‐organic heterostructures provide a versatile and scalable material platform for the development of next‐generation neuromorphic systems and adaptive optoelectronic applications.