Gold‐Template‐Assisted Mechanical Exfoliation of Large‐Area 2D Layers Enables Efficient and Precise Construction of Moiré Superlattices

Abstract Moiré superlattices, consisting of rotationally aligned 2D atomically thin layers, provide a highly novel platform for the study of correlated quantum phenomena. However, reliable and efficient construction of moiré superlattices is challenging because of difficulties to accurately angle‐align small exfoliated 2D layers and the need to shun wet‐transfer processes. Here, efficient and precise construction of various moiré superlattices is demonstrated by picking up and stacking large‐area 2D mono‐ or few‐layer crystals with predetermined crystal axes, made possible by a gold‐template‐assisted mechanical exfoliation method. The exfoliated 2D layers are semiconductors, superconductors, or magnets and their high quality is confirmed by photoluminescence and Raman spectra and by electrical transport measurements of fabricated field‐effect transistors and Hall devices. Twisted homobilayers with angle‐twisting accuracy of ≈0.3°, twisted heterobilayers with sub‐degree angle‐alignment accuracy, and multilayer superlattices are precisely constructed and characterized by their moiré patterns, interlayer excitons, and second harmonic generation. The present study paves the way for exploring emergent phenomena in moiré superlattices.