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Graphene nanoribbons grown in hBN stacks for high-performance electronics

Nature volume 628, pages 758–764 (2024)Cite this article

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Abstract

Van der Waals encapsulation of two-dimensional materials in hexagonal boron nitride (hBN) stacks is a promising way to create ultrahigh-performance electronic devices1,2,3,4. However, contemporary approaches for achieving van der Waals encapsulation, which involve artificial layer stacking using mechanical transfer techniques, are difficult to control, prone to contamination and unscalable. Here we report the transfer-free direct growth of high-quality graphene nanoribbons (GNRs) in hBN stacks. The as-grown embedded GNRs exhibit highly desirable features being ultralong (up to 0.25 mm), ultranarrow (<5 nm) and homochiral with zigzag edges. Our atomistic simulations show that the mechanism underlying the embedded growth involves ultralow GNR friction when sliding between AA′-stacked hBN layers. Using the grown structures, we demonstrate the transfer-free fabrication of embedded GNR field-effect devices that exhibit excellent performance at room temperature with mobilities of up to 4,600 cm2 V–1 s–1 and on–off ratios of up to 106. This paves the way for the bottom-up fabrication of high-performance electronic devices based on embedded layered materials.

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Fig. 1: Directly grown embedded graphene nanoribbons.
Fig. 2: Ultralong embedded zigzag GNRs exhibiting 1D moiré superstructures.
Fig. 3: Embedded GNR sliding mechanism.
Fig. 4: Superior FETs based on the embedded GNRs.

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Data availability

The data supporting the findings of this study are available in this paper and its Supplementary Information or from the corresponding authors upon request.

Code availability

The codes related to the findings of this study are available from the corresponding authors upon request.

Change history

  • 28 March 2024

    A production error introduced in the title of the scale bar in Fig. 4b was corrected from Isd to |Isd| (A).

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Acknowledgements

This work is supported by the National Key R&D Program of China (no. 2021YFA1202902, 2020YFA0309000, 2022YFA1405400 and 2022YFA1402702), the National Natural Science Foundation of China (no. 12374292, 12074244, 12102307, 11890673, 11890674, 11874258, 12074247, 12174249 and 92265102), the open research fund of Songshan Lake Materials Laboratory (no. 2021SLABFK07). W.O. acknowledges the Natural Science Foundation of Hubei Province (2021CFB138) and the start-up fund of Wuhan University. M.U. acknowledges the financial support from the Israel Science Foundation (grant no. 1141/18) and the ISF-NSFC joint grant 3191/19. O.H. is grateful for the financial support from the Israel Science Foundation (grant no. 1586/17), Tel Aviv University Center for Nanoscience and Nanotechnology, the Naomi Foundation by the 2017 Kadar Award and the Heineman Chair of Physical Chemistry. Shiyong Wang acknowledges support from the Shanghai Municipal Science and Technology Qi Ming Xing Project (no. 20QA1405100) and the Fok Ying Tung Foundation for young researchers. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan, (grant no. JPMXP0112101001), JSPS KAKENHI (grant nos. 19H05790 and 20H00354) and A3 Foresight by JSPS. Shiyong Wang and Z.S. acknowledge support from the Shanghai Jiao Tong University (21X010200846) and further support from the Shanghai talent program. L.Q. acknowledges the support from the Basic Research Laboratory Support Program (grant no. 2021R1A4A1033224) of the National Research Foundation of Korea. B.L. acknowledges support from the Development Scholarship for Outstanding Ph.D. of Shanghai Jiao Tong University. We also acknowledge support from the Instrument Analysis Center of Shanghai Jiao Tong University for performing focused ion beam application on GAIA3 and STEM on TALOS F200X. Molecular dynamics simulations were carried out at the National Supercomputer TianHe-1(A) Center in Tianjin and the Supercomputing Center of Wuhan University.

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Author notes

  1. These authors contributed equally: Bosai Lyu, Jiajun Chen, Sen Wang, Shuo Lou, Peiyue Shen, Jingxu Xie, Lu Qiu, Izaac Mitchell

Authors and Affiliations

  1. Key Laboratory of Artificial Structures and Quantum Control (Ministry of Education), Shenyang National Laboratory for Materials Science, School of Physics and Astronomy, Shanghai Jiao Tong University, Shanghai, China

    Bosai Lyu, Jiajun Chen, Shuo Lou, Peiyue Shen, Jingxu Xie, Can Li, Cheng Hu, Xianliang Zhou, Xiaoqun Wang, Jinfeng Jia, Qi Liang, Guorui Chen, Tingxin Li, Shiyong Wang & Zhiwen Shi

  2. Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, China

    Bosai Lyu, Jiajun Chen, Shuo Lou, Peiyue Shen, Jingxu Xie, Can Li, Cheng Hu, Xianliang Zhou, Xiaoqun Wang, Jinfeng Jia, Qi Liang, Shiyong Wang & Zhiwen Shi

  3. Department of Engineering Mechanics, School of Civil Engineering, Wuhan University, Wuhan, China

    Sen Wang & Wengen Ouyang

  4. State Key Laboratory of Water Resources and Hydropower Engineering Science, Wuhan University, Wuhan, China

    Sen Wang & Wengen Ouyang

  5. Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology, Ulsan, South Korea

    Lu Qiu, Izaac Mitchell & Feng Ding

  6. Graduate School of Carbon Neutrality, Ulsan National Institute of Science and Technology, Ulsan, South Korea

    Lu Qiu

  7. Department of Mechanical Engineering, Ulsan National Institute of Science and Technology, Ulsan, South Korea

    Lu Qiu

  8. Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, Japan

    Kenji Watanabe

  9. International Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan

    Takashi Taniguchi

  10. Tsung-Dao Lee Institute, Shanghai Jiao Tong University, Shanghai, China

    Xiaoqun Wang, Jinfeng Jia, Qi Liang, Tingxin Li, Shiyong Wang & Zhiwen Shi

  11. Department of Physical Chemistry, School of Chemistry and The Sackler Center for Computational Molecular and Materials Science, The Raymond and Beverly Sackler Faculty of Exact Sciences, Tel Aviv University, Tel Aviv, Israel

    Oded Hod & Michael Urbakh

  12. Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China

    Feng Ding

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Contributions

B.L. and Z.S. initiated the project. Z.S., M.U., F.D., O.H. and W.O. supervised the project. B.L., J.C. and S.L. grew the samples. J.C. and B.L. carried out the TEM and STEM measurements. B.L., J.C. and P.S. carried out the SEM measurements. B.L., J.C. and S.L. carried out the AFM measurements. P.S., B.L. and J.C. fabricated the devices and conducted the electron transport measurements. Sen Wang and J.X. conducted the molecular dynamics simulations of GNR sliding. W.O. designed the molecular dynamics simulation setup and implemented the codes. L.Q., I.M. and F.D. carried out the theoretical calculations. K.W. and T.T. grew the hBN single crystals. B.L., J.C., S.L., Sen Wang, P.S., L.Q., I.M., C.L., C.H., X.Z., W.O., J.X., X.W., J.J., Q.L., Shiyong Wang, G.C., T.L., M.U., O.H., F.D. and Z.S. analysed the data. B.L., J.C., Sen Wang, S.L., L.Q., I.M., W.O., M.U., O.H., F.D. and Z.S. wrote the paper with input from all the authors.

Corresponding authors

Correspondence to Wengen Ouyang, Feng Ding, Michael Urbakh or Zhiwen Shi.

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Extended data figures and tables

Extended Data Fig. 1 AFM topography images of embedded GNRs and Fe nanoparticles at hBN step edges.

a, 3D AFM topography image of hBN step edges after Fe nanoparticle deposition and CVD growth. b, Zoom-in on the region marked by the dashed square in panel (a) demonstrating an embedded-GNR grown from a nanoparticle into the hBN stack. c and d, AFM topography images of hBN step edges with high nanoparticle density. e, Height profile taken along the blue dashed line in panels (c) and (d).

Extended Data Fig. 2 Demonstration of CVD growth of embedded GNRs.

a, SEM image of a bare hBN sample prior to growth. b, SEM image of the same sample as in panel a, following CVD growth. The bright lines are SEM fingerprints of embedded GNRs grown from edge-positioned catalytic nanoparticles.

Extended Data Fig. 3 Removal of on-surface GNRs through plasma etching.

Upper two panels are AFM topography images captured at the same hBN surface region following CVD growth, before a and after b plasma etching, respectively. Panels c and d present a schematic view of panels a and b, respectively.

Extended Data Fig. 4 Additional cross-sectional STEM images of embedded GNRs.

a, A large-scale STEM side-view image showing two embedded GNRs. b-e, Zoom-in STEM images. f-j, High-resolution STEM images of five embedded-GNRs with width in the range from 3 nm to 5 nm. k, Width statistics. Scale bar: (a) 20 nm, (b-e) 3 nm, (f-j) 2 nm.

Extended Data Fig. 5 Large-scale SEM images of embedded GNRs.

Straight embedded-GNRs of typical length of a few tens of micrometers mostly oriented along three distinct directions on the hBN flake that are angularly separated by 60o. Scale bar: (a) 5 μm, (b) 30 μm, (c) 20 μm and (d) 40 μm.

Extended Data Fig. 6 Transfer and output characteristics of additional GNR devices.

a-f, Room temperature transfer and output characteristics of six devices with channel lengths ranging from 1 μm to 30.7 μm. See SI section 7 for a discussion of the oscillations observed in the transfer curves.

Extended Data Fig. 7 Estimation of mobility and subthreshold swing of GNR devices.

a, Room temperature transfer characteristics (black) of a GNR device of channel length of L ≈ 24 μm, width of ≈3 nm, and SiO2 thickness of 285 nm (Cgs = 10 pF/m). A linear fit (red dashed line) yields a carrier mobility of ≈4,600 cm2V–1s–1. b, Room temperature transfer characteristics (black) of a different device (L ≈ 8 μm, width of ≈3 nm, and SiO2 thickness of 285 nm, Cgs = 10 pF/m), demonstrating a carrier mobility of ≈2,155 cm2 V–1 s–1. c and d, Carrier mobility as a function of gate voltage extracted from the transfer characteristics of the devices shown in panel (a) and (b), respectively. e, The statistics of carrier mobility. Semi-log plots of the transfer characteristic curves of a (f) 17 μm and (g) 8 μm long channel devices (≈3 nm in width) demonstrating similar room temperature subthreshold swing values of ≈ 100 mV/dec, as extracted from the slope of the dashed grey lines.

Extended Data Fig. 8 Temperature-dependent carrier mobility.

a, Transfer characteristics of a high-performance device at Vsd = 0.5 V for different temperatures. b, Measured mobility as a function of temperature. Inset: the measured mobility as a function of \({T}^{-1}\) (black squares) and the corresponding linear fit.

Extended Data Fig. 9 Representative types of inter-ribbon architectures.

Three-dimensional AFM height images (upper panels) and schematic illustrations (lower panels) of (a) vertically parallel, (b) vertically crossed, and (c) intersected planar Y-junction GNR architectures. For clarity, the top hBN layers are hidden in the three schematic illustrations.

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Lyu, B., Chen, J., Wang, S. et al. Graphene nanoribbons grown in hBN stacks for high-performance electronics. Nature 628, 758–764 (2024). https://doi.org/10.1038/s41586-024-07243-0

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  • DOI: https://doi.org/10.1038/s41586-024-07243-0

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