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Epitaxial growth of wafer-scale molybdenum disulfide semiconductor single crystals on sapphire

Abstract

Two-dimensional (2D) semiconductors, in particular transition metal dichalcogenides (TMDCs), have attracted great interest in extending Moore’s law beyond silicon1,2,3. However, despite extensive efforts4,5,6,7,8,9,10,11,12,13,14,15,16,17,18,19,20,21,22,23,24,25, the growth of wafer-scale TMDC single crystals on scalable and industry-compatible substrates has not been well demonstrated. Here we demonstrate the epitaxial growth of 2 inch (~50 mm) monolayer molybdenum disulfide (MoS2) single crystals on a C-plane sapphire. We designed the miscut orientation towards the A axis (C/A) of sapphire, which is perpendicular to the standard substrates. Although the change of miscut orientation does not affect the epitaxial relationship, the resulting step edges break the degeneracy of nucleation energy for the antiparallel MoS2 domains and lead to more than a 99% unidirectional alignment. A set of microscopies, spectroscopies and electrical measurements consistently showed that the MoS2 is single crystalline and has an excellent wafer-scale uniformity. We fabricated field-effect transistors and obtained a mobility of 102.6 cm2 V−1 s−1 and a saturation current of 450 μA μm–1, which are among the highest for monolayer MoS2. A statistical analysis of 160 field-effect transistors over a centimetre scale showed a >94% device yield and a 15% variation in mobility. We further demonstrated the single-crystalline MoSe2 on C/A sapphire. Our method offers a general and scalable route to produce TMDC single crystals towards future electronics.

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Fig. 1: Sapphire (0001) substrate and epitaxial relationship.
Fig. 2: Unidirectional alignment of MoS2 domains on a C/A sapphire (0001) substrate.
Fig. 3: Mechanism of unidirectional nucleation.
Fig. 4: Wafer-scale MoS2 single crystals.
Fig. 5: FET performance.

Data availability

The data that support the findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

This work is supported by the Natural Science Foundation of Jiangsu Province (grant no. BK20202005), the National Key R&D Program of China (grant no. 2017YFA0204800), National Natural Science Foundation of China (grant nos 61927808, 61521001, 61734003, 61851401, 91964202, 61861166001, 51861145202; 51972162, 22033002, 21525311, 21903014, 11774153 and 11874199), Strategic Priority Research Program of the Chinese Academy of Sciences XDB 30000000, Key Laboratory of Advanced Photonic and Electronic Materials, Collaborative Innovation Center of Solid-State Lighting and Energy-Saving Electronics and the Fundamental Research Funds for the Central Universities, China.

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Contributions

X.W. conceived and supervised the project. T.L. performed the CVD growth with assistance from L.L., Z.W., Y. Yang, W. Lin and N.D., and guidance from Y. Yao and Y.S. W.G. and Y.N. performed the RHEED, LEED and XRD characterizations and data analysis. L.M. and J.W. performed the density functional theory calculations. Z.H., S.G. and P.W. performed the TEM and data analysis. X.C. and Z.L. contributed to the spectral characterizations, including PL, Raman spectroscopy and SHG mapping. Z.Y., W. Li, D.F., X.T. and D.P. contributed to transistor fabrication, measurements and data analysis. T.L., J.W. and X.W. co-wrote the manuscript with input from other authors. All the authors contributed to discussions.

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Correspondence to Jinlan Wang or Xinran Wang.

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Peer review information Nature Nanotechnology thanks Xiangfeng Duan, Joan Redwing and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–21, Table 1 and References.

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Li, T., Guo, W., Ma, L. et al. Epitaxial growth of wafer-scale molybdenum disulfide semiconductor single crystals on sapphire. Nat. Nanotechnol. (2021). https://doi.org/10.1038/s41565-021-00963-8

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