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Abstract For hardware artificial intelligence, the central task is to design and develop artificial synapses with needed characteristics. Here, the design and experimental demonstration of a van der Waals (vdW) photo‐ferroelectric synapse are reported. In the photo‐ferroelectric synapse, the synaptic memory is extracted by reading the photocurrent, and written or edited by electrical pulses. The semiconducting vdW organic‐inorganic halide perovskite ((R)‐(–)‐1‐cyclohexylethylammonium)PbI₃(R‐CYHEAPbI₃) photo‐ferroelectric serves as the model photo‐ferroelectric channel. Here, the vdW organic layer provides ferroelectric dipole and the PbI₆octahedron is responsible for photon absorption and charge transport. The R‐CYHEAPbI₃photo‐ferroelectric synapse show a writing/reading dynamics with >200 synaptic states, close to 10³on/off ratio, and reasonable endurance and retention characteristics. With the experimentally measured weight dynamics (parallel reading through ferroelectric photovoltaic effect and writing by electrical pulses) of R‐CYHEAPbI₃synapses, the feasibility of using a crossbar circuit to implement classic training and inference of hand‐written digits is presented. An image recognition accuracy of up to 90% is obtained. The demonstration of such a vdW photo‐ferroelectric synapse opens a window in the design of advanced devices for artificial intelligence. 

Abstract The ability to reconfigure spin structure and spin‐photon interactions by an external electric field is a prerequisite for seamless integration of opto‐spintronics into modern electronics. In this study, the use of electric field on the tuning of circular photo galvanic effect in a quasi‐2D oxyhalide perovskite Bi₄NbO₈Cl is reported. The electrical transport measurements are applied to study the switching characteristics of the microsheet devices. The electric field is used to tune the nanoscale devices and an optical orientation approach is applied to understand the field‐tuned spin‐polarized band structures. It is found that the circular photogalvanic current can be erased and re‐created by poling, indicating the electric‐field‐based control over spin structure. The study enriches the basic understanding of the symmetry‐regulated optoelectronic response in ferroelectrics with spin‐orbit coupling.