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Designed growth of large bilayer graphene with arbitrary twist angles

Nature Materials volume 21, pages 1263–1268 (2022)Cite this article

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Abstract

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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Fig. 1: Schematic for the growth design of TBG.
Fig. 2: Twist-angle replication from the rotated Cu foils.
Fig. 3: Characterizations of TBG.
Fig. 4: Angle tunability in TBG.

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Data availability

Source data are provided with this paper. All other data that support the findings of this study are available within the Article and the Supplementary Information.

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Acknowledgements

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.

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Author notes

  1. These authors contributed equally: Can Liu, Zehui Li, Ruixi Qiao, Qinghe Wang.

Authors and Affiliations

  1. State Key Laboratory for Mesoscopic Physics, Frontiers Science Center for Nano-optoelectronics, School of Physics, Peking University, Beijing, China

    Can Liu, Zehui Li, Qinghe Wang, Zhibin Zhang, Fang Liu, Ziqi Zhou, Nianze Shang, Zuo Feng, Yang Cheng, Dewei Gong, Hao Hong, Xinqiang Wang & Kaihui Liu

  2. Department of Physics, Renmin University of China, Beijing, China

    Can Liu

  3. International Centre for Quantum Materials, Collaborative Innovation Centre of Quantum Matter, Peking University, Beijing, China

    Ruixi Qiao, Muhong Wu, Peng Gao, Enge Wang & Kaihui Liu

  4. Institute for Frontier Science, Nanjing University of Aeronautics and Astronautics, Nanjing, China

    Ruixi Qiao

  5. ShanghaiTech Laboratory for Topological Physics, School of Physical Science and Technology, Shanghai Tech University, Shanghai, China

    Hongwei Fang, Meixiao Wang, Zhongkai Liu & Zhu-Jun Wang

  6. State Key Laboratory of Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences, Beijing, China

    Heng Wu & Ping-Heng Tan

  7. Shenzhen Institute for Quantum Science and Engineering, Southern University of Science and Technology, Shenzhen, China

    Song Liu, Zhensheng Zhang, Dingxin Zou & Dapeng Yu

  8. Songshan Lake Materials Laboratory, Institute of Physics, Chinese Academy of Sciences, Dongguan, China

    Ying Fu & Enge Wang

  9. Key Laboratory of Artificial Micro- and Nano-structures of Ministry of Education, School of Physics and Technology, Wuhan University, Wuhan, China

    Jun He

  10. Interdisciplinary Institute of Light-Element Quantum Materials and Research Center for Light-Element Advanced Materials, Peking University, Beijing, China

    Muhong Wu

  11. School of Physics, Liaoning University, Shenyang, China

    Enge Wang

Authors
  1. Can Liu
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Contributions

K.L., Z.-J.W. and C.L. conceived the project. C.L., Z. Li and Q.W. performed the growth experiments. Z. Li and R.Q. conducted the equipotential surface etching experiments. Q.W., Z. Zhang, F.L. and X.W. performed the EBSD and XRD measurements. R.Q., P.G. and D.Y. performed the HRTEM and SAED experiments. C.L., Y.C., H.W., H.H. and P.-H.T. conducted the optical characterizations. Z. Zhou, N.S. and Z.F. performed the photocurrent measurements. H.F., M. Wang and Z. Liu conducted the ARPES characterizations. D.G., D.Z. and M. Wu contributed to the preparation of Cu(111) single crystals. Important contributions to the interpretation of the results and conception were made by K.L., C.L. and Z.-J.W. All the authors revised and commented on the paper.

Corresponding authors

Correspondence to Can Liu, Zhu-Jun Wang or Kaihui Liu.

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Liu, C., Li, Z., Qiao, R. et al. Designed growth of large bilayer graphene with arbitrary twist angles. Nat. Mater. 21, 1263–1268 (2022). https://doi.org/10.1038/s41563-022-01361-8

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