High‐Performance Memristors Based on Few‐Layer Manganese Phosphorus Trisulfide for Neuromorphic Computing

Abstract While transition‐metal thiophosphate (MPX 3 ) materials have been a subject of extensive research in recent years, experimental studies on MPX 3 ‐based memristors are still in their early stages, with device performance being less than ideal. Here, the successful fabrication of high‐yield, high‐performance, and uniform memristors are demonstrated to possess desired characteristics for neuromorphic computing using a single‐crystalline few‐layered manganese phosphorus trisulfide (MnPS 3 ) as a resistive switching medium. The Ti/MnPS 3 /Au memristor exhibits small switching voltage (<1 V), long memory retention (10 4 s), fast switching speed (≈20 ns), high On/Off ratio (nearly two orders of magnitude), and simultaneously achieves emulation of synaptic weight plasticity. The microscopic investigation of the structural and chemical characteristics of the few‐layer MnPS 3 reveals the presence of structural defects and residual Ti throughout the stacked layer following the application of voltage, which contributes to the uniformity of switching with a low set voltage. With highly linear and symmetric analog weight updates coupled with the capability of accurate decimal arithmetic operations, a high accuracy of 95.15% in supervised learning using the MNIST handwritten recognition dataset is achieved in the artificial neural network. Furthermore, convolutional image processing can be implemented using hardware multiply‐and‐accumulate operation in an experimental memristor crossbar array.