Programmable Optoelectronic Synaptic Transistors Based on MoS₂/Ta₂NiS₅ Heterojunction for Energy‐Efficient Neuromorphic Optical Operation

Abstract The optoelectronic synaptic transistors with various functions, broad spectral perception, and low power consumption are an urgent need for the development of advanced optical neural network systems. However, it remains a great challenge to realize the functional diversification of the systems on a single device. 2D van der Waals (vdW) materials can combine unique properties by stacking with each other to form heterojunctions, which may provide a strategy for solving this problem. Herein, an all‐2D vdW heterojunction‐based programmable optoelectronic synaptic transistor based on MoS₂/Ta₂NiS₅ heterojunctions is demonstrated. The device implements reconfigurable, multilevel non‐volatile memory (NVM) states through sequential modulation of multiple optical and electrical stimuli to achieve broadband (532–808 nm), energy‐efficient (17.2 fJ), hetero‐synaptic functionality in a bionic manner. The intrinsic working mechanisms of the photogating effect caused by band alignment and the interfacial trapping defect modulation induced by gate voltage are revealed by Kelvin‐probe force microscopy (KPFM) measurements and carrier transport analysis. Overall, the (opto)electronic synaptic weight controllability for combined in‐sensor and in‐memory logic processors is realized by the heterojunction properties. The proposed findings facilitate the technical realization of generic all 2D hetero‐synapses for future artificial vision systems, opto‐logical systems, and Internet of Things (IoT) entities.