Reversible writing of high-mobility and high-carrier-density doping patterns in two-dimensional van der Waals heterostructures

Abstract

A key feature of two-dimensional materials is that the sign and concentration of their carriers can be externally controlled with techniques such as electrostatic gating. However, conventional electrostatic gating has limitations, including a maximum carrier density set by the dielectric breakdown, and ionic liquid gating and direct chemical doping also suffer from drawbacks. Here, we show that an electron-beam-induced doping technique can be used to reversibly write high-resolution doping patterns in hexagonal boron nitride-encapsulated graphene and molybdenum disulfide (MoS2) van der Waals heterostructures. The doped MoS2 device exhibits an order of magnitude decrease of subthreshold swing compared with the device before doping, whereas the doped graphene devices demonstrate a previously inaccessible regime of high carrier concentration and high mobility, even at room temperature. We also show that the approach can be used to write high-quality p–n junctions and nanoscale doping patterns, illustrating that the technique can create nanoscale circuitry in van der Waals heterostructures.

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Fig. 1: Electron-beam-induced doping effect in graphene and MoS2 vdW heterostructures.
Fig. 2: Energy dependence of electron-beam-induced doping effect in graphene and MoS2 vdW heterostructures.
Fig. 3: Transport characteristics and spatially controlled nanoscale doping patterns of BN/Gr/BN heterostructures by electron-beam-induced doping.
Fig. 4: Energy dependence and proposed mechanism for the electron-beam-induced doping effect in graphene and MoS2 vdW heterostructures.

Data availability

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

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Acknowledgements

We thank Y. Chen, W. Ruan, S. Zhao, and J. Jung for useful discussions. This work was supported in part by the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, and Molecular Foundry of the US Department of Energy under contract no. DE-AC02-05-CH11231, primarily within the van der Waals Heterostructures Program (KCWF16), which provided for development of the concept and device fabrication, electron-beam doping and transport characterization, and within the sp2-Bonded Materials Program (KC2207), which provided for s-SNOM measurements, and by the National Science Foundation, under grant no.1542741, which provided for AFM topography and SdH measurements, and under grant no.1807233, which provided for EFM measurements.

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A.Z., M.C., W.S., S.K., H.-Z.T. and D.W. conceived the experiment. S.K., W.S. and S.-Y.W. contributed to device fabrication. W.S. and S.K. performed all electrical measurements, EFM measurements and data analysis. K.W. and T.T. provided the BN crystals. L.J. and F.W. contributed to the s-SNOM measurements. W.S., S.K. and A.Z. co-wrote the manuscript, with inputs and comments from all authors.

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Correspondence to Alex Zettl.

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Supplementary Information

Supplementary Notes 1–18, Figs. 1–27 and Table 1.

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Shi, W., Kahn, S., Jiang, L. et al. Reversible writing of high-mobility and high-carrier-density doping patterns in two-dimensional van der Waals heterostructures. Nat Electron 3, 99–105 (2020). https://doi.org/10.1038/s41928-019-0351-x

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