Van der Waals Assembly of Multilayer Twisted Transition Metal Dichalcogenides With Controllable Chirality

Abstract Transition metal dichalcogenides (TMDCs) bilayer moiré superlattices exhibit remarkable properties in valley spin polarization, nonlinear optics, and circular polarization optics. Despite these advancements, the exploration of multilayer twisted TMDCs systems remains limited due to the significant challenge in achieving twisting controllable, large‐area fabrication with high stacking quality. Here, an efficient assembly method is presented for constructing continuous multilayer twisted TMDCs homojunctions and heterojunctions, leveraging the rapid decoupling and recombination of van der Waals (vdW) forces on TMDCs surfaces. This approach is not only time‐efficient but also enables large‐area transfer with clean vdW interfaces. Furthermore, the successful stacking of multilayer twisted TMDCs films with helical chirality is demonstrated using achiral building blocks, elucidating the structure‐activity relationships among chirality, twist angle, and layer number. The work not only provides an efficient method to precisely prepare multilayer twisted TMDCs, but also establishes a robust framework for investigating the novel properties and structure‐activity relationships in complex TMDCs systems.