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Just as biological synapses provide basic functions for the nervous system, artificial synaptic devices serve as the fundamental building blocks of neuromorphic networks; thus, developing novel artificial synapses is essential for neuromorphic computing. By exploiting the band alignment between 2D inorganic and organic semiconductors, the first multi-functional synaptic transistor based on a molybdenum disulfide (MoS 2 )/perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) hybrid heterojunction, with remarkable short-term plasticity (STP) and longterm plasticity (LTP), is reported. Owing to the elaborate design of the energy band structure, both robust electrical and optical modulation are achieved through carriers transfer at the interface of the heterostructure, which is still a challenging task to this day. In electrical modulation, synaptic inhibition and excitation can be achieved simultaneously in the same device by gate voltage tuning. Notably, a minimum inhibition of 3% and maximum facilitation of 500% can be obtained by increasing the electrical number, and the response to different frequency signals indicates a dynamic filtering characteristic. It exhibits flexible tunability of both STP and LTP and synaptic weight changes of up to 60, far superior to previous work in optical modulation. The fully 2D MoS 2 /PTCDA hybrid heterojunction artificial synapse opens up a whole new path for the urgent need for neuromorphic computation devices.

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