Non-volatile resistive switching, also known as memristor effect in two terminal devices, has emerged as one of the most important components in the ongoing development of high-density information storage, brain-inspired computing, and reconfigurable systems. Recently, the unexpected discovery of memristor effect in atomic monolayers of transitional metal dichalcogenide sandwich structures has added a new dimension of interest owing to the prospects of size scaling and the associated benefits. However, the origin of the switching mechanism in atomic sheets remains uncertain. Here, using monolayer MoS$_2$ as a model system, atomistic imaging and spectroscopy reveal that metal substitution into sulfur vacancy results in a non-volatile change in resistance. The experimental observations are corroborated by computational studies of defect structures and electronic states. These remarkable findings provide an atomistic understanding on the non-volatile switching mechanism and open a new direction in precision defect engineering, down to a single defect, for achieving optimum performance metrics including memory density, switching energy, speed, and reliability using atomic nanomaterials.
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