The great potential of artificial optoelectronic devices that are capable of mimicking biosynapse functions in brain-like neuromorphic computing applications has aroused extensive interest, and the architecture design is decisive yet challenging. Herein, a new architecture of p-type CuZnSnS@BiOBr nanosheets embedded in poly(methyl methacrylate) (PMMA) films (CZTS@BOB-PMMA) is presented acting as a switching layer, which not only shows the bipolar resistive switching features (SET/RESET voltages, ∼ -0.93/+1.35 V; retention, >10 s) and electrical- and near-infrared light-induced synapse plasticity but also demonstrates electrical-driven excitatory postsynaptic current, spiking-time-dependent plasticity, paired pulse facilitation, long-term plasticity, long- and short-term memory, and "learning-forgetting-learning" behaviors. The approach is a rewarding attempt to broaden the research of optoelectric controllable memristive devices for building neuromorphic architectures mimicking human brain functionalities.
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