Giant Photoluminescence Enhancement and Carrier Dynamics in MoS₂ Bilayers with Anomalous Interlayer Coupling

Fundamental researches and explorations based on transition metal dichalcogenides (TMDCs) mainly focus on their monolayer counterparts, where optical densities are limited owing to the atomic monolayer thickness. Photoluminescence (PL) yield in bilayer TMDCs is much suppressed owing to indirect-bandgap properties. Here, optical properties are explored in artificially twisted bilayers of molybdenum disulfide (MoS2). Anomalous interlayer coupling and resultant giant PL enhancement are firstly observed in MoS2 bilayers, related to the suspension of the top layer material and independent of twisted angle. Moreover, carrier dynamics in MoS2 bilayers with anomalous interlayer coupling are revealed with pump-probe measurements, and the secondary rising behavior in pump-probe signal of B-exciton resonance, originating from valley depolarization of A-exciton, is firstly reported and discussed in this work. These results lay the groundwork for future advancement and applications beyond TMDCs monolayers