Air-stable lithiation engineering of MoS₂ for direct-bandgap multilayers

Due to its sizable direct bandgap and strong light-matter interactions, the preparation of monolayer $\mathrm{MoS}_{2}$ has attracted significant attention and intensive research efforts. However, multilayer $\mathrm{MoS}_{2}$ is largely overlooked because of its optically inactive indirect bandgap caused by interlayer coupling. It is highly desirable to modulate and decrease the interlayer coupling so that each layer in multilayer $\mathrm{MoS}_{2}$ can exhibit a monolayer-like direct-gap behavior. Here, we demonstrate the nanoprobe fabrication of $\mathrm{Li}_{x}\mathrm{MoS}_{2}$-based multilayers exhibiting a direct bandgap and strong photoluminescence emission from tightly bound excitons and trions. The fabrication is facilitated by our newly developed Li-ion platform, featuring tip-induced Li intercalation, air stability and rewritability. Raman characterizations reveal that controlled Li intercalation effectively transforms multilayer $\mathrm{MoS}_{2}$ into the stack of multiple monolayers, leading to a 26-fold enhancement of photoluminescence, compared to a monolayer. This intercalation result is different from existing observations of transforming $\mathrm{MoS}_{2}$ multilayers into metallic phases.