Wavelength‐Controlled Photoconductance Polarity Switching via Harnessing Defects in Doped PdSe₂ for Artificial Synaptic Features

Abstract Optoelectronic synapses are currently drawing significant attention as fundamental building blocks of neuromorphic computing to mimic brain functions. In this study, a two‐terminal synaptic device based on a doped PdSe₂ flake is proposed to imitate the key neural functions in an optical pathway. Due to the wavelength‐dependent desorption of oxygen clusters near the intrinsic selenide vacancy defects, the doped PdSe₂ photodetector achieves a high negative photoresponsivity of −7.8 × 10³ A W⁻¹ at 473 nm and a positive photoresponsivity of 181 A W⁻¹ at 1064 nm. This wavelength‐selective bi‐direction photoresponse endows an all‐optical pathway to imitate the fundamental functions of artificial synapses on a device level, such as psychological learning and forgetting capability, as well as dynamic logic functions. The underpinning photoresponse is further demonstrated on a flexible platform, providing a viable technology for neuromorphic computing in wearable electronics. Furthermore, the p‐type doping results in an effective increase of the channel's electrical conductivity and a significant reduction in power consumption. Such low‐power‐consuming optical synapses with simple device architecture and low‐dimensional features demonstrate tremendous promise for building multifunctional artificial neuromorphic systems in the future.