Reliable Memristor Crossbar Array Based on 2D Layered Nickel Phosphorus Trisulfide for Energy‐Efficient Neuromorphic Hardware

Abstract Designing reliable and energy‐efficient memristors for artificial synaptic arrays in neuromorphic computing beyond von Neumann architecture remains a challenge. Here, memristors based on emerging layered nickel phosphorus trisulfide (NiPS 3 ) are reported that exhibit several favorable characteristics, including uniform bipolar nonvolatile switching with small operating voltage (<1 V), fast switching speed (< 20 ns), high On/Off ratio (>10 2 ), and the ability to achieve programmable multilevel resistance states. Through direct experimental evidence using transmission electron microscopy and energy dispersive X‐ray spectroscopy, it is revealed that the resistive switching mechanism in the Ti/NiPS 3 /Au device is related to the formation and dissolution of Ti conductive filaments. Intriguingly, further investigation into the microstructural and chemical properties of NiPS 3 suggests that the penetration of Ti ions is accompanied by the drift of phosphorus‐sulfur ions, leading to induced P/S vacancies that facilitate the formation of conductive filaments. Furthermore, it is demonstrated that the memristor, when operating in quasi‐reset mode, effectively emulates long‐term synaptic weight plasticity. By utilizing a crossbar array, multipattern memorization and multiply‐and‐accumulate (MAC) operations are successfully implemented. Moreover, owing to the highly linear and symmetric multiple conductance states, a high pattern recognition accuracy of ≈96.4% is demonstrated in artificial neural network simulation for neuromorphic systems.