2D-layered materials are recognized as up-and-coming candidates to overcome the intrinsic physical limitation of silicon-based devices. Herein, the coexistence of positive persistent photoconductivity (PPPC) and negative persistent photoconductivity (NPPC) in SnSe thin films prepared by pulsed laser deposition provides an excellent avenue for engineering novel devices. It is determined that surface oxygen is co-regulated by physisorption and chemisorption, and the NPPC is attributed to the photo-controllable oxygen desorption behavior. The dominant behavior of chemisorption induces high stability, while physisorption provides room for adjusting NPPC. A simple fully light-modulated artificial synaptic device based on SnSe film is constructed to operate various synaptic plasticity and reversible modulation of conductance by applying 430 and 255nm illuminations. A three-layer artificial neural network structure with a high accuracy of 95.33% to recognize handwritten digital images is implemented based on the device. Furthermore, the pressure-related cognition response of humans while climbing and the foraging and recognition behaviors of anemonefish are mimicked. This work demonstrates the potential of 2D-layered materials for developing neuromorphic computing and simulating biological behaviors without additional treatment. Furthermore, the one-step method for preparation is highly adaptable and expected to realize large-area growth and integration of SnSe-based devices.
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