Spatially Dependent Electronic Structures and Excitons in a Marginally Twisted Moiré Superlattice of Spiral WS₂

Twisted two-dimensional transition metal dichalcogenide (TMD) moiré superlattices provide an additional degree of freedom to engineer electronic and optical properties. Nevertheless, controllable synthesis of marginally twisted homo TMD moiré superlattices is still a challenge. Here, physical vapor deposition grown spiral WS₂ nanosheets are demonstrated to be a marginally twisted moiré superlattice using scanning tunneling microscopy and spectroscopy. Periodic moiré superlattices are found on the third layer (3L) and 4L of the spiral WS₂ nanosheet owing to the marginally twisted alignment between two neighboring layers, resulting in a highly localized flat band near the valence band maximum. Their bandgap depends on atomic stacking configurations, which gives a good interpretation for split moiré excitons using photoluminescence at 77 K. This work can benefit the development of twisted homo TMD moiré superlattices and could promote the profound research of twisted TMDs in the prospective field, such as strongly correlated physics and twistronics.