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A wafer-scale van der Waals dielectric made from an inorganic molecular crystal film

Abstract

Van der Waals dielectrics, such as hexagonal boron nitride, are widely used to preserve the intrinsic properties of two-dimensional semiconductors in electronic devices. However, fabricating these materials on the wafer scale and integrating them with two-dimensional semiconductors is challenging because their synthesis typically requires mechanical exfoliation or vapour deposition processes. Here we show that a high-κ van der Waals dielectric can be created on wafer scales using an inorganic molecular crystal film of antimony trioxide (Sb2O3) fabricated via thermal evaporation deposition. Monolayer molybdenum disulfide (MoS2) field-effect transistors supported by this dielectric substrate exhibit enhanced electron mobility—from 26 cm2 V−1 s−1 to 145 cm2 V−1 s−1—and reduced transfer-curve hysteresis compared with when using SiO2 substrate. MoS2 transistors directly gated by the Sb2O3 film can operate with a supply voltage of 0.8 V, on/off ratio of 108 and subthreshold swing of 64 mV dec−1 at 300 K.

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Fig. 1: Fabrication of a wafer-scale Sb2O3 film via STED.
Fig. 2: Dielectric properties of Sb2O3 film.
Fig. 3: MoS2 FET supported by vdW Sb2O3 substrate.
Fig. 4: Hysteresis of MoS2 FETs supported on Sb2O3 and SiO2 substrates.
Fig. 5: Top-gated MoS2 FETs using Sb2O3 as the gate dielectric.

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Data availability

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

References

  1. Radisavljevic, B., Radenovic, A., Brivio, J., Giacometti, V. & Kis, A. Single-layer MoS2 transistors. Nat. Nanotechnol. 6, 147–150 (2011).

    Article  Google Scholar 

  2. Li, L. et al. Black phosphorus field-effect transistors. Nat. Nanotechnol. 9, 372–377 (2014).

    Article  Google Scholar 

  3. Kang, K. et al. High-mobility three-atom-thick semiconducting films with wafer-scale homogeneity. Nature 520, 656–660 (2015).

    Article  Google Scholar 

  4. Liu, Y., Duan, X., Huang, Y. & Duan, X. Two-dimensional transistors beyond graphene and TMDCs. Chem. Soc. Rev. 47, 6388–6409 (2018).

    Article  Google Scholar 

  5. Aljarb, A. et al. Ledge-directed epitaxy of continuously self-aligned single-crystalline nanoribbons of transition metal dichalcogenides. Nat. Mater. 19, 1300–1306 (2020).

    Article  Google Scholar 

  6. Dean, C. R. et al. Boron nitride substrates for high-quality graphene electronics. Nat. Nanotechnol. 5, 722–726 (2010).

    Article  Google Scholar 

  7. Rhodes, D., Chae, S. H., Ribeiro-Palau, R. & Hone, J. Disorder in van der Waals heterostructures of 2D materials. Nat. Mater. 18, 541–549 (2019).

    Article  Google Scholar 

  8. Wang, L. et al. One-dimensional electrical contact to a two-dimensional material. Science 342, 614–617 (2013).

    Article  Google Scholar 

  9. Cui, X. et al. Multi-terminal transport measurements of MoS2 using a van der Waals heterostructure device platform. Nat. Nanotechnol. 10, 534–540 (2015).

    Article  Google Scholar 

  10. Cadiz, F. et al. Excitonic linewidth approaching the homogeneous limit in MoS2-based van der Waals heterostructures. Phys. Rev. X 7, 021026 (2017).

    Google Scholar 

  11. Cao, Y. et al. Unconventional superconductivity in magic-angle graphene superlattices. Nature 556, 43–50 (2018).

    Article  Google Scholar 

  12. Lee, G. et al. Flexible and transparent MoS2 field-effect transistors on hexagonal boron nitride-graphene heterostructures. ACS Nano 7, 7931–7936 (2013).

    Article  Google Scholar 

  13. Lee, G.-H. et al. Highly stable, dual-gated MoS2 transistors encapsulated by hexagonal boron nitride with gate-controllable contact, resistance, and threshold Voltage. ACS Nano 9, 7019–7026 (2015).

    Article  Google Scholar 

  14. Xue, J. et al. Scanning tunnelling microscopy and spectroscopy of ultra-flat graphene on hexagonal boron nitride. Nat. Mater. 10, 282–285 (2011).

    Article  Google Scholar 

  15. Decker, R. et al. Local electronic properties of graphene on a BN substrate via scanning tunneling microscopy. Nano Lett. 11, 2291–2295 (2011).

    Article  Google Scholar 

  16. Kim, S. M. et al. Synthesis of large-area multilayer hexagonal boron nitride for high material performance. Nat. Commun. 6, 8662 (2015).

    Article  Google Scholar 

  17. Chen, T. A. et al. Wafer-scale single-crystal hexagonal boron nitride monolayers on Cu (111). Nature 579, 219–223 (2020).

    Article  Google Scholar 

  18. Illarionov, Y. et al. Ultrathin calcium fluoride insulators for two-dimensional field-effect transistors. Nat. Electron. 2, 230–235 (2019).

    Article  Google Scholar 

  19. Wang, L. et al. Epitaxial growth of a 100-square-centimetre single-crystal hexagonal boron nitride monolayer on copper. Nature 570, 91–95 (2019).

    Article  Google Scholar 

  20. Svensson, C. Refinement of the crystal structure of cubic antimony trioxide, Sb2O3. Acta Crystallogr. B 31, 2016–2018 (1975).

    Article  Google Scholar 

  21. Pereira, A. L. J. et al. Structural and vibrational study of cubic Sb2O3 under high pressure. Phys. Rev. B 85, 174108 (2012).

    Article  Google Scholar 

  22. Han, W. et al. Two-dimensional inorganic molecular crystals. Nat. Commun. 10, 4728 (2019).

    Article  Google Scholar 

  23. Zhou, Y. et al. Thin-film Sb2Se3 photovoltaics with oriented one-dimensional ribbons and benign grain boundaries. Nat. Photon. 9, 409–415 (2015).

    Article  Google Scholar 

  24. Wang, Y. et al. Van der Waals contacts between three-dimensional metals and two-dimensional semiconductors. Nature 568, 70–74 (2019).

    Article  Google Scholar 

  25. Late, D. J. et al. Hysteresis in single-layer MoS2 field effect transistors. ACS Nano 6, 5635–5641 (2012).

    Article  Google Scholar 

  26. Liu, Y., Stradins, P. & Wei, S.-H. Van der Waals metal–semiconductor junction: weak Fermi level pinning enables effective tuning of Schottky barrier. Sci. Adv. 2, e1600069 (2016).

    Article  Google Scholar 

  27. Amit, I. et al. Role of charge traps in the performance of atomically thin transistors. Adv. Mater. 29, 1605598 (2017).

    Article  Google Scholar 

  28. Lee, C.-H. et al. Atomically thin p–n junctions with van der Waals heterointerfaces. Nat. Nanotechnol. 9, 676–681 (2014).

    Article  Google Scholar 

  29. Illarionov, Y. Y. et al. The role of charge trapping in MoS2/SiO2 and MoS2/hBN field-effect transistors. 2D Mater. 3, 035004 (2016).

    Article  Google Scholar 

  30. McDonnell, S. et al. HfO2 on MoS2 by atomic layer deposition: adsorption mechanisms and thickness scalability. ACS Nano 7, 10354–10361 (2013).

    Article  Google Scholar 

  31. Li, W. et al. Uniform and ultrathin high-κ gate dielectrics for two-dimensional electronic devices. Nat. Electron. 2, 563–571 (2019).

    Article  Google Scholar 

  32. Datye, I. M. et al. Reduction of hysteresis in MoS2 transistors using pulsed voltage measurements. 2D Mater. 6, 011004 (2019).

    Article  Google Scholar 

  33. Illarionov, Y. Y. et al. Improved hysteresis and reliability of MoS2 transistors with high-quality CVD growth and Al2O3 encapsulation. IEEE Electron Device Lett. 12, 1763–1766 (2017).

    Google Scholar 

  34. Jung, Y. et al. Transferred via contacts as a platform for ideal two-dimensional transistors. Nat. Electron. 2, 187–194 (2019).

    Article  Google Scholar 

  35. Li, T. et al. A native oxide high-κ gate dielectric for two-dimensional electronics. Nat. Electron. 3, 473–478 (2020).

    Article  Google Scholar 

  36. Knobloch, T. et al. The performance limits of hexagonal boron nitride as an insulator for scaled CMOS devices based on two-dimensional materials. Nat. Electron. 4, 98–108 (2021).

    Article  Google Scholar 

  37. Britnell, L. et al. Field-effect tunneling transistor based on vertical graphene heterostructures. Science 335, 947–950 (2012).

    Article  Google Scholar 

  38. Ju, L. et al. Photoinduced doping in heterostructures of graphene and boron nitride. Nat. Nanotechnol. 9, 348–352 (2014).

    Article  Google Scholar 

  39. Vu, Q. A. et al. Two-terminal floating-gate memory with van der Waals heterostructures for ultrahigh on/off ratio. Nat. Commun. 7, 12725 (2016).

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Nature Science Foundation of China (21825103, 51727809 and 11904154), the Hubei Provincial Nature Science Foundation of China (2019CFA002) and the Fundamental Research Funds for the Central Universities (2019kfyXMBZ018). We also acknowledge the Analytical and Testing Center of Huazhong University of Science and Technology for the TEM characterizations and analysis. Computational time is partially supported by the Center for Computational Science and Engineering of Southern University of Science and Technology. We thank X. Shi (Hebei University) and B. Deng (Shenzhen JL Computational Science and Applied Research Institute) for the fruitful discussions about the theoretical calculations. We also appreciate the inspiring discussions with S. Hu and Y. Cao (Xiamen University).

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Contributions

K.L. and T.Z. conceived the ideas. K.L. and B.J. designed and carried out most of the experiments under T.Z.’s supervision. K.L., B.J. and X.H. deposited the film. K.L. and J.D. performed the measurement of the absorption spectrum. P.G. and L.H. carried out the first-principles calculations. X.C., L. Li., S.Y. and F.Z. helped to analyse the data. K.L., W.H., L. Liu. and T.Z. worked on the images with assistance from all the others. K.L. wrote the paper with inputs from all the authors.

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Correspondence to Tianyou Zhai.

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

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Supplementary Figs. 1–23 and Tables 1–5.

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Liu, K., Jin, B., Han, W. et al. A wafer-scale van der Waals dielectric made from an inorganic molecular crystal film. Nat Electron 4, 906–913 (2021). https://doi.org/10.1038/s41928-021-00683-w

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