Ultra‐Large‐Period Moiré Lattices in Twisted Trilayer MoS ₂ Induced by High‐Symmetry Sites

Abstract

ABSTRACT Twisted trilayer (Tt) transition metal dichalcogenides with multiple rotational degrees of freedom offer unprecedented opportunities for constructing large‐wavelength moiré superlattices to maximize the effect of correlated behaviors. Precisely stacking trilayer structures to realize ultra‐large moiré superlattices remains a significant challenge, hindering investigations of moiré‐tuned excitonic properties. Here we fabricate Tt MoS 2 via chemical vapor deposition, in which two commensurate twists of 2.7° and 21.9° are sequentially introduced from the top to middle, and to bottom layers. An unprecedented super‐moiré structure with an ultra‐large periodicity of around 24 nm is achieved, 30 times larger than that of 21.9°‐bilayer MoS 2 , hierarchically composed of periodical mirror‐symmetric triangular tessellation patterns consisting of five kinds of high‐symmetric stacking registrations and the relaxation regions resulting from the interlayer gliding. This robust ultra‐large‐period superstructure generates a deep moiré potential to effectively suppress intralayer moiré excitons recombination and be against intervalley exchange interaction at the magnetic field up to 9T, associated with the enhanced layer‐valley‐locked polarization by two‐fold larger than that of the trilayer systems with incommensurate angles. Our work presents angle‐dependent super‐moiré architectures in Tt systems as a versatile platform for designing moiré quantum materials with tailored optoelectronic responses, advancing applications in valleytronic and excitonic devices.