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Large transport gap modulation in graphene via electric-field-controlled reversible hydrogenation

Nature Electronics volume 4, pages 254–260 (2021)Cite this article

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Abstract

Graphene is of interest in the development of next-generation electronics due to its high electron mobility, flexibility and stability. However, graphene transistors have poor on/off current ratios because of the absence of a bandgap. One approach to introduce an energy gap is to use a hydrogenation reaction, which changes graphene into insulating graphane with sp3 bonding. Here we show that an electric field can be used to control the conductor-to-insulator transitions in microscale graphene via reversible electrochemical hydrogenation in an organic liquid electrolyte containing dissociative hydrogen ions. The fully hydrogenated graphene exhibits a lower sheet resistance limit of 200 GΩ sq−1, resulting in graphene field-effect transistors with on/off current ratios of 108 at room temperature. The devices also exhibit high endurance, with up to 1 million switching cycles. Similar insulating behaviours are also observed in bilayer graphene, while trilayer graphene remains highly conductive after hydrogenation. Changes in the graphene lattice, and the transformation from sp2 to sp3 hybridization, are confirmed by in situ Raman spectroscopy, supported by first-principles calculations.

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Fig. 1: Electric-field control of reversible hydrogenation in MLG.
Fig. 2: Characterization of the insulating and switching behaviours of hydrogenated MLG.
Fig. 3: Electric-field control of reversible hydrogenation in BLG and TLG.
Fig. 4: DFT calculations of hydrogenated MLG, BLG and TLG.

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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

We thank Y. Xu for helpful discussions and technical support. This work is supported by the Basic Science Center Project of NSFC (grant no. 51788104) and the National Key R&D Program of China (grant nos. 2018YFA0307100 and 2016YFA0301001). This work is supported in part by the Beijing Advanced Innovation Center for Future Chips (ICFC).

Author information

Author notes

  1. These authors contributed equally: Shaorui Li, Jiaheng Li, Yongchao Wang.

Authors and Affiliations

  1. State Key Laboratory of Low-Dimensional Quantum Physics, Department of Physics, Tsinghua University, Beijing, China

    Shaorui Li, Jiaheng Li, Chenglin Yu, Yaoxin Li, Wenhui Duan, Yayu Wang & Jinsong Zhang

  2. Beijing Innovation Center for Future Chips, Tsinghua University, Beijing, China

    Yongchao Wang

  3. Institute for Advanced Study, Tsinghua University, Beijing, China

    Wenhui Duan

  4. Frontier Science Center for Quantum Information, Beijing, China

    Wenhui Duan, Yayu Wang & Jinsong Zhang

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  1. Shaorui Li
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Contributions

J.S.Z. and Y.Y.W. proposed and supervised the research. J.S.Z. designed the device structure and proposed the electrolyte. S.R.L., Y.C.W., C.L.Y. and Y.X.L. fabricated the devices and carried out the electric measurements. S.R.L. and Y.C.W. measured the Raman spectra. W.H.D. and J.H.L. performed the theoretical calculations. J.S.Z., Y.Y.W. and S.R.L. prepared the manuscript with comments from all the authors.

Corresponding authors

Correspondence to Yayu Wang or Jinsong Zhang.

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Peer review information Nature Electronics thanks Cody Hayashi and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Li, S., Li, J., Wang, Y. et al. Large transport gap modulation in graphene via electric-field-controlled reversible hydrogenation. Nat Electron 4, 254–260 (2021). https://doi.org/10.1038/s41928-021-00548-2

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