The production of large-area twisted bilayer graphene (TBG) with controllable angles is a prerequisite for proceeding with its massive applications. However, most of the prevailing strategies to fabricate twisted bilayers face great challenges, where the transfer methods are easily stuck by interfacial contamination, and direct growth methods lack the flexibility in twist-angle design. Here we develop an effective strategy to grow centimetre-scale TBG with arbitrary twist angles (accuracy, <1.0°). The success in accurate angle control is realized by an angle replication from two prerotated single-crystal Cu(111) foils to form a Cu/TBG/Cu sandwich structure, from which the TBG can be isolated by a custom-developed equipotential surface etching process. The accuracy and consistency of the twist angles are unambiguously illustrated by comprehensive characterization techniques, namely, optical spectroscopy, electron microscopy, photoemission spectroscopy and photocurrent spectroscopy. Our work opens an accessible avenue for the designed growth of large-scale two-dimensional twisted bilayers and thus lays the material foundation for the future applications of twistronics at the integration level.
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This work was supported by Guangdong Major Project of Basic and Applied Basic Research with grant no. 2021B0301030002 (E.W. and K.L.); Beijing Natural Science Foundation under grant no. JQ19004 (K.L.); the National Natural Science Foundation of China under grant nos. 52025023 (K.L.), 51991342 (K.L.), 52021006 (K.L.), 11888101 (E.W.), 92163206 (M. Wu), 12027804 (Z.-J.W.), 52172035 (M. Wu), 52100115 (Z. Li), 52125307 (P.G.) and T2188101 (K.L.); the National Key R&D Program of China under grant nos. 2021YFB3200303 (K.L.), 2021YFA1400201 (H.H.), 2021YFA1400502 (M. Wu) and 2018YFA0703700 (J.H.); the Key R&D Program of Guangdong Province under grant nos. 2020B010189001 (K.L.), 2019B010931001 (K.L.) and 2018B030327001 (D.Y.); the Strategic Priority Research Program of Chinese Academy of Sciences with grant no. XDB33000000 (K.L.); the Pearl River Talent Recruitment Program of Guangdong Province with grant no. 2019ZT08C321 (K.L.). We acknowledge the Electron Microscopy Laboratory in Peking University for use of the electron microscope.
The authors declare no competing interests.
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Liu, C., Li, Z., Qiao, R. et al. Designed growth of large bilayer graphene with arbitrary twist angles. Nat. Mater. (2022). https://doi.org/10.1038/s41563-022-01361-8