Nondefective Vacancy Enhanced Resistive Switching Reliability in Emergent van der Waals Metal Phosphorus Trisulfide-Based Memristive In-Memory Computing Hardware.

Two-dimensional-material-based memristors are emerging as promising enablers of new computing systems beyond von Neumann computers. However, the most studied anion-vacancy-enabled transition metal dichalcogenide memristors show many undesirable performances, e.g., high leakage currents, limited memory windows, high programming currents, and limited endurance. Here, we demonstrate that the emergent van der Waals metal phosphorus trisulfides with unconventional nondefective vacancy provide a promising paradigm for high-performance memristors. The different vacancy types (i.e., defective and nondefective vacancies) induced memristive discrepancies are uncovered. The nondefective vacancies can provide an ultralow diffusion barrier and good memristive structure stability giving rise to many desirable memristive performances, including high off-state resistance of 10 12 Ω, pA-level programming currents, large memory window up to 10 9 , more than 7-bit conductance states, and good endurance. Furthermore, a high-yield (94%) memristor crossbar array is fabricated and implements multiple image processing successfully, manifesting the potential for in-memory computing hardware.