Macroscopic Uniform 2D Moiré Superlattices with Controllable Angles

Moiré superlattices, engineered through precise stacking of van der Waals (vdW) layers, hold immense promise for exploring strongly correlated and topological phenomena. However, these applications have been held back by the common preparation method: tear-and-stack of Scotch tape exfoliated monolayers, which suffer from low efficiency and reproducibility, twist angle inhomogeneity, interfacial contamination, and micrometer sizes. Here, we report an effective strategy to construct highly consistent mixed-dimensional and twisted bilayer vdW moiré structures with high production throughput, near-unity yield, pristine interfaces, precisely controlled twist angles, and macroscopic scale (up to centimeters) with enhanced thermal stability. We demonstrate the versatility across various vdW materials, including transition metal dichalcogenides, graphene, and hBN. The expansive size and high quality of moiré structures enable reciprocal-space high-resolution mapping of the superlattices and back-folded moiré mini band structures with low energy electron diffraction (LEED) and angle-resolved photoemission spectroscopy (ARPES). In particular, we identify the backfolded bands at the K point of twisted transition metal dichalcogenide moiré structures. This technique will have broad applications in both fundamental studies and the mass production of twistronic devices.