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Sub-10-nm graphene nanoribbons with atomically smooth edges from squashed carbon nanotubes

Nature Electronics volume 4, pages 653–663 (2021)Cite this article

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Abstract

Graphene nanoribbons are of potential use in the development of electronic and optoelectronic devices. However, the preparation of narrow and long nanoribbons with smooth edges, sizeable bandgaps and high mobilities is challenging. Here we show that sub-10-nm-wide semiconducting graphene nanoribbons with atomically smooth closed edges can be produced by squashing carbon nanotubes using a high-pressure and thermal treatment. With this approach, nanoribbons as narrow as 1.4 nm can be created, and up to 54% of single- and double-walled nanotubes in a sample can be converted into edge-closed nanoribbons. We also fabricate edge-opened nanoribbons using nitric acid as the oxidant to selectively etch the edges of the squashed nanotubes under high pressure. A field-effect transistor fabricated using a 2.8-nm-wide edge-closed nanoribbon exhibits an on/off current ratio of more than 104, from which a bandgap of around 494 meV is estimated. The device also exhibits a field-effect mobility of 2,443 cm2 V−1 s−1 and an on-state channel conductivity of 7.42 mS.

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Fig. 1: In situ Raman measurements of the samples undergoing a high-pressure and thermal treatment in a DAC.
Fig. 2: TEM and STEM images of GNRs from squashed CNTs.
Fig. 3: High-resolution STEM characterization of GNRs in treated Samples 1 and 2 and a DWCNT.
Fig. 4: Edge-opened GNRs with the edges selectively etched by HNO3 at high pressure.
Fig. 5: AFM images and Raman measurements of edge-closed GNRs from squashed CNTs.
Fig. 6: Room-temperature electrical measurements of an edge-closed GNR from a squashed DWCNT.

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Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

C.C. acknowledges support from the National Natural Science Foundation of China for Excellent Young Scholars (no. 61622404), Chang Jiang (Cheung Kong) Scholars Program of Ministry of Education of China (no. Q2017081), National Natural Science Foundation of China (no. 62074098) and Science and Technology Innovation Action Program from the Science and Technology Commission of Shanghai Municipality (no. 15520720200). Y.L., W.L.M. and the high-pressure DAC experiments were supported by the United States Department of Energy through the Stanford Institute for Materials and Energy Sciences DE-AC02-76SF00515. Work by J.N.W. was supported by the National Key R&D Program of China (2018YFA0208404) and Innovation Program of Shanghai Municipal Education Commission. J.G. was supported by NSF grant nos. 1809770 and 1904580. Work at ORNL was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. W.Z. acknowledges support from the Beijing Outstanding Young Scientist Program (BJJWZYJH01201914430039).

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Author notes

  1. These authors contributed equally: Changxin Chen, Yu Lin, Wu Zhou.

Authors and Affiliations

  1. National Key Laboratory of Science and Technology on Micro/Nano Fabrication, Key Laboratory for Thin Film and Microfabrication of Ministry of Education, Department of Micro/Nano Electronics, School of Electronic Information and Electrical Engineering, Shanghai Jiao Tong University, Shanghai, China

    Changxin Chen, Zhuoyang He, Fangyuan Shi & Xinyue Li

  2. Department of Chemistry, Stanford University, Stanford, CA, USA

    Changxin Chen, Ming Gong, Justin Zachary Wu, Guosong Hong, Alexander L. Antaris & Hongjie Dai

  3. Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Yu Lin & Wendy L. Mao

  4. Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA

    Wu Zhou

  5. School of Physical Sciences and CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing, China

    Wu Zhou

  6. Department of Electrical and Computer Engineering, University of Florida, Gainesville, FL, USA

    Kai Tak Lam & Jing Guo

  7. School of Materials Science and Engineering, East China University of Science and Technology, Shanghai, China

    Jian Nong Wang

  8. Department of Geological Sciences, Stanford University, Stanford, CA, USA

    Fan Yang & Wendy L. Mao

  9. Center for High Pressure Science and Technology Advanced Research, Shanghai, China

    Qiaoshi Zeng

  10. Jiangsu Key Laboratory of Advanced Metallic Materials, School of Materials Science and Engineering, Southeast University, Nanjing, China

    Qiaoshi Zeng

  11. Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign, Urbana, IL, USA

    Wenpei Gao & Jian-Min Zuo

  12. Department of Chemistry, Duke University, Durham, NC, USA

    Jie Liu

  13. College of Electrical Engineering and Automation, Shandong University of Science and Technology, Qingdao, China

    Meng-Chang Lin

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Contributions

H.D. and C.C. conceived and designed the experiments and C.C. conceived the theoretical calculations and simulations. C.C. planned and supervised the project. C.C., Y.L., W.Z., M.G., Z.H., F.S., X.L., J.Z.W., J.N.W., F.Y., Q.Z., J.L., G.H., A.L.A. and M.-C.L. performed the experiments and prepared the pristine CNT samples. C.C., Z.H., K.T.L., J.G., W.G. and J.-M.Z. performed the numerical simulations. C.C., Y.L., W.Z., M.G., Z.H., F.S., X.L., J.Z.W., K.T.L., F.Y., Q.Z., J.G., W.G., J.-M.Z., G.H., W.L.M. and H.D. analysed the data and wrote the manuscript. All the authors discussed the results and commented on the manuscript.

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Correspondence to Changxin Chen, Wendy L. Mao or Hongjie Dai.

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Peer review information Nature Electronics thanks Antonio Pantano, Chee-Tat Toh and An-Ping Li for their contribution to the peer review of this work.

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Supplementary Figs. 1–20, Table 1 and Notes 1–3.

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Chen, C., Lin, Y., Zhou, W. et al. Sub-10-nm graphene nanoribbons with atomically smooth edges from squashed carbon nanotubes. Nat Electron 4, 653–663 (2021). https://doi.org/10.1038/s41928-021-00633-6

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