Twist-angle-dependent momentum-space direct and indirect interlayer excitons in WSe₂/WS₂ heterostructure

Interlayer excitons (ILEs) in the van der Waals (vdW) heterostructures of type-II band alignment transition metal dichalcogenides (TMDCs) have attracted significant interest owing to their unique exciton properties and potential in quantum information applications. However, the new dimension that emerges with the stacking of structures with a twist angle leads to a more complex fine structure of ILEs, presenting both an opportunity and a challenge for the regulation of the interlayer excitons. In this study, we report the evolution of interlayer excitons with the twist angle in the WSe₂/WS₂ heterostructure and identify the direct (indirect) interlayer excitons by combining photoluminescence (PL) and density functional theory (DFT) calculations. Two interlayer excitons with opposite circular polarization assigned to the different transition paths of K-K and Q-K were observed. The nature of the direct (indirect) interlayer exciton was confirmed by circular polarization PL measurement, excitation power-dependent PL measurement and DFT calculations. Furthermore, by applying an external electric field to regulate the band structure of the WSe₂/WS₂ heterostructure and control the transition path of the interlayer excitons, we could successfully realize the regulation of interlayer exciton emission. This study provides more evidence for the twist-angle-based control of heterostructure properties.