Making Patterned Single Defects in MoS₂ Thermally with the MoS₂/Au Moiré Interface

Normally, it is hard to regulate thermal defects precisely in their host lattice due to the stochastic nature of thermal activation. Here, we demonstrate a thermal annealing way to create patterned single sulfur vacancy (V_S) defects in monolayer molybdenum disulfide (MoS₂) with about 2 nm separations at subnanometer accuracy. Theoretically, we reveal that the S-Au interface coupling reduces the energy barriers in forming V_S defects and that explains the overwhelming formation of interface V_S defects. We also discover a phonon regulation mechanism by the moiré interface that effectively condenses the Γ-point out-of-plane acoustic phonons of monolayer MoS₂ to its TOP moiré sites, which has been proposed to trigger moiré-patterned thermal V_S formation. The high-throughput nanoscale patterned defects presented here may contribute to building scalable defect-based quantum systems.