In Situ Growth of High‐Quality Single‐Crystal Twisted Bilayer Graphene on Liquid Copper

Abstract Twisted bilayer graphene (TBG) generates significant attention in the fundamental research of 2D materials due to its distinct twist‐angle‐dependent properties. Exploring the efficient production of TBG with a wide range of twist angles stands as one of the major frontiers in moiré materials. Here, the local space‐confined chemical vapor deposition growth technique for high‐quality single‐crystal TBG with twist angles ranging from 0° to 30° on liquid copper substrates is reported. The clean surface, pristine interface, high crystallinity, and thermal stability of TBG are verified by using comprehensive characterization techniques including optical microscopy, electron microscopy, and secondary‐ion mass spectrometry. The proportion of TBG in bilayer graphene reaches as high as 89%. In addition, the stacking structure and growth mechanism of TBG are investigated, revealing that the second graphene layer develops beneath the first one. A series of comparative experiments illustrates that the liquid copper surface, with its excellent fluidity, promotes the growth of TBG. Electrical measurements show the twist‐angle‐dependent electronic properties of as‐grown TBG, achieving a room‐temperature carrier mobility of 26640 cm² V⁻¹ s⁻¹. This work provides an approach for the in situ preparation of 2D twisted materials and facilitates the application of TBG in the fields of electronics.