One‐Interlayer‐Twisted Multilayer MoS2 Moiré Superlattices

Abstract Twist angle provides a new degree of freedom for 2D material modifications. In principle, the intrinsic properties of twisted multilayers can be regulated by twist angle between each adjacent layer and thus have greater tunability than widely studied bilayer structures. Considering its complexity, it is important to first investigate the simplest twisted multilayers with only one interface twisted. In this work, multilayer Moiré superlattices with only one twisted interface via paraffin‐assisted folding of non‐twisted stacked (highly symmetrically stacked) multilayer MoS 2 are successfully fabricated, and their twist‐angle dependent optical properties are systematically studied. Compared to non‐twisted stacked multilayer MoS 2 , the one‐interface‐twisted multilayers show a 2–3.5 times higher PL intensity, and their interlayer coupling, indirect bandgap, and degree of circular polarization (DOCP) are tunable by twist angle. Notably, the DOCP for the one‐interface‐twisted four‐layer (folded bilayer) can reach 86%, which is the highest value ever reported for transition metal dichalcogenide homostructures above liquid nitrogen temperature. This work provides a solid base for understanding twist‐angle dependent properties of twisted multilayer 2D‐materials.