Intrinsic Defect‐Driven Synergistic Synaptic Heterostructures for Gate‐Free Neuromorphic Phototransistors

Abstract The optoelectronic synaptic devices based on two‐dimensional (2D) materials offer great advances for future neuromorphic visual systems with dramatically improved integration density and power efficiency. The effective charge capture and retention are considered as one vital prerequisite to realizing the synaptic memory function. However, the current 2D synaptic devices are predominantly relied on materials with artificially‐engineered defects or intricate gate‐controlled architectures to realize the charge trapping process. These approaches, unfortunately, suffer from the degradation of pristine materials, rapid device failure, and unnecessary complication of device structures. To address these challenges, an innovative gate‐free heterostructure paradigm is introduced herein. The heterostructure presents a distinctive dome‐like morphology wherein a defect‐rich Fe₇S₈ core is enveloped snugly by a curved MoS₂ dome shell (Fe₇S₈@MoS₂), allowing the realization of effective photocarrier trapping through the intrinsic defects in the adjacent Fe₇S₈ core. The resultant neuromorphic devices exhibit remarkable light‐tunable synaptic behaviors with memory time up to ≈800 s under single optical pulse, thus demonstrating great advances in simulating visual recognition system with significantly improved image recognition efficiency. The emergence of such heterostructures foreshadows a promising trajectory for underpinning future synaptic devices, catalyzing the realization of high‐efficiency and intricate visual processing applications.