Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Vertically grown metal nanosheets integrated with atomic-layer-deposited dielectrics for transistors with subnanometre capacitance-equivalent thicknesses

Abstract

Integrating thin atomic-layer-deposited dielectrics with two-dimensional (2D) semiconductors could be used to fabricate 2D transistors with sub-1 nm capacitance-equivalent thicknesses. However, non-uniform nucleation from atomic-layer deposition on inert surfaces and subsequent high-energy metal evaporation can make atomically thin dielectrics non-insulating. Here, we report a bismuth-oxide-assisted chemical vapour deposition method to synthesize single-crystalline metal nanosheets with atomically flat surfaces. The nanosheets grow vertically on a substrate and can be easily transferred to a target substrate through polymer-free mechanical pressing. We show that palladium nanosheets offer an excellent surface for atomic-layer deposition of flat aluminium oxide (Al2O3) and hafnium oxide (HfO2) dielectrics with sub-3 nm thicknesses. These can then be laminated onto few-layer molybdenum disulfide (MoS2) as a gate stack with a capacitance-equivalent thickness of 0.9 nm and a capacitance density of around 3.9 μF cm−2. Our MoS2 top-gated transistors with a 2-nm-thick Al2O3 or HfO2 dielectric exhibit leakage currents of 10−6 A cm−2, low operating voltages of around 0.45 V and a hysteresis of less than 1 mV.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: CVD growth, polymer-free transfer and characterizations of vertically grown single-crystalline metals.
Fig. 2: ALD compatibility and vdW integration of vertically grown Pd nanosheets.
Fig. 3: MoS2 transistors with sub-3 nm Al2O3/Pd as top-gate dielectric and electrode.
Fig. 4: MoS2 transistors with 2 nm HfO2/Pd based as top-gate dielectric and electrode.

Similar content being viewed by others

Data availability

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

References

  1. Li, W. et al. Approaching the quantum limit in two-dimensional semiconductor contacts. Nature 613, 274–279 (2023).

    Article  Google Scholar 

  2. Tan, C. et al. 2D fin field-effect transistors integrated with epitaxial high-k gate oxide. Nature 616, 66–72 (2023).

    Article  Google Scholar 

  3. Jiang, J. Ballistic two-dimensional InSe transistors. Nature 616, 470–475 (2023).

    Article  Google Scholar 

  4. Liu, Y. et al. Promises and prospects of two-dimensional transistors. Nature 591, 43–53 (2021).

    Article  Google Scholar 

  5. Desai, S. B. et al. MoS2 transistors with 1-nanometer gate lengths. Science 354, 99–102 (2016).

    Article  Google Scholar 

  6. Lin, Y. C. et al. Dielectric material technologies for 2D semiconductor transistor scaling. IEEE Trans. Electron Devices 70, 1454–1473 (2023).

    Article  Google Scholar 

  7. Yang, S. et al. Gate dielectrics integration for 2D electronics: challenges, advances, and outlook. Adv. Mater. 35, 2207901 (2023).

    Article  Google Scholar 

  8. Illarionov, Y. Y. et al. Insulators for 2D nanoelectronics: the gap to bridge. Nat. Commun. 11, 3385 (2020).

    Article  Google Scholar 

  9. Das, S. et al. Transistors based on two-dimensional materials for future integrated circuits. Nat. Electron. 4, 786–799 (2021).

    Article  Google Scholar 

  10. Wang, S. et al. Two-dimensional devices and integration towards the silicon lines. Nat. Mater. 21, 1225–1239 (2022).

    Article  Google Scholar 

  11. Badaroglu, M. International Roadmap for Devices and Systems (IEEE, 2021).

  12. Wong, H. et al. On the scaling of subnanometer EOT gate dielectrics for ultimate nano CMOS technology. Microelectron. Eng. 138, 57–76 (2015).

    Article  Google Scholar 

  13. Huang, J. et al. High-κ perovskite membranes as insulators for two-dimensional transistors. Nature 605, 262–267 (2022).

    Article  Google Scholar 

  14. Luo, P. et al. Molybdenum disulfide transistors with enlarged van der Waals gaps at their dielectric interface via oxygen accumulation. Nat. Electron. 5, 849–858 (2022).

    Article  Google Scholar 

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

    Article  Google Scholar 

  16. Kim, H. G. et al. Atomic layer deposition on 2D materials. Chem. Mater. 29, 3809–3826 (2017).

    Article  Google Scholar 

  17. 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 

  18. 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 

  19. Xu, Y. et al. Scalable integration of hybrid high-κ dielectric materials on two-dimensional semiconductors. Nat. Mater. 22, 1078–1084 (2023).

    Article  Google Scholar 

  20. Wang, X. et al. Improved integration of ultra-thin high-k dielectrics in few-layer MoS2 FET by remote forming gas plasma pretreatment. Appl. Phys. Lett. 110, 53110 (2017).

    Article  Google Scholar 

  21. Park, J. H. et al. Atomic layer deposition of Al2O3 on WSe2 functionalized by titanyl phthalocyanine. ACS Nano 10, 6888–6896 (2016).

    Article  Google Scholar 

  22. Liu, Y. et al. Approaching the Schottky–Mott limit in van der Waals metal-semiconductor junctions. Nature 557, 696–700 (2018).

    Article  Google Scholar 

  23. Yang, X. et al. Highly reproducible van der Waals integration of two-dimensional electronics on the wafer scale. Nat. Nanotechnol. 18, 471–478 (2023).

    Article  Google Scholar 

  24. Liu, G. et al. Graphene-assisted metal transfer printing for wafer-scale integration of metal electrodes and two-dimensional materials. Nat. Electron. 5, 275–280 (2022).

    Article  Google Scholar 

  25. Wang, L. et al. A general one-step plug-and-probe approach to top-gated transistors for rapidly probing delicate electronic materials. Nat. Nanotechnol. 17, 1206–1213 (2022).

    Article  Google Scholar 

  26. Lu, Z. et al. Wafer-scale high-κ dielectrics for two-dimensional circuits via van der Waals integration. Nat. Commun. 14, 2340 (2023).

    Article  Google Scholar 

  27. Chen, J. et al. Vertically grown ultrathin Bi2SiO5 as high-κ single-crystalline gate dielectric. Nat. Commun. 14, 4406 (2023).

    Article  Google Scholar 

  28. Zhang, C. et al. Single-crystalline van der Waals layered dielectric with high dielectric constant. Nat. Mater. 22, 832–837 (2023).

    Article  Google Scholar 

  29. Jin, Y. et al. Controllable oxidation of ZrS2 to prepare high-κ, single-crystal m-ZrO2 for 2D electronics. Adv. Mater. 35, 2212079 (2023).

    Article  Google Scholar 

  30. Wang, J. et al. Transferred metal gate to 2D semiconductors for sub-1 V operation and near ideal subthreshold slope. Sci. Adv. 7, f8744 (2021).

    Article  Google Scholar 

  31. Yang, A. J. et al. Van der Waals integration of high-κ perovskite oxides and two-dimensional semiconductors. Nat. Electron. 5, 233–240 (2022).

    Article  Google Scholar 

  32. Sharma, V. K. et al. Single atom catalyst-mediated generation of reactive species in water treatment. Chem. Soc. Rev. 52, 7673–7686 (2023).

    Article  Google Scholar 

  33. Fan, Z. et al. Thin metal nanostructures: synthesis, properties and applications. Chem. Sci. 6, 95–111 (2015).

    Article  Google Scholar 

  34. Jiang, J. et al. Van der Waals epitaxy growth of 2D single-element room-temperature ferromagnet. Adv. Mater. 35, 2211701 (2023).

    Article  Google Scholar 

  35. Li, W. et al. Free-standing 2D ironene with magnetic vortex structure at room temperature. Matter 5, 291–301 (2022).

    Article  Google Scholar 

  36. Qin, B. et al. General low-temperature growth of two-dimensional nanosheets from layered and nonlayered materials. Nat. Commun. 14, 304 (2023).

    Article  Google Scholar 

  37. Zhou, J. et al. Composition and phase engineering of metal chalcogenides and phosphorous chalcogenides. Nat. Mater. 22, 450–458 (2023).

    Article  Google Scholar 

  38. Zhao, Z. et al. A general thermodynamics-triggered competitive growth model to guide the synthesis of two-dimensional nonlayered materials. Nat. Commun. 14, 958 (2023).

    Article  Google Scholar 

  39. Zhou, J. et al. A library of atomically thin metal chalcogenides. Nature 556, 355–359 (2018).

    Article  Google Scholar 

  40. Hong, C. et al. Inclined ultrathin Bi2O2Se films: a building block for functional van der Waals heterostructures. ACS Nano 14, 16803–16812 (2020).

    Article  Google Scholar 

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

    Article  Google Scholar 

  42. Mondal, A. et al. Low ohmic contact resistance and high on/off ratio in transition metal dichalcogenides field-effect transistors via residue-free transfer. Nat. Nanotechnol. 19, 34–43 (2024).

    Article  Google Scholar 

  43. Fleetwood, D. M. Border traps’ in MOS devices. IEEE T. Nucl. Sci. 39, 269–271 (1992).

    Article  Google Scholar 

  44. Knobloch, T. et al. A physical model for the hysteresis in MoS2 transistors. IEEE J. Electron Device 6, 972–978 (2018).

    Article  Google Scholar 

  45. Illarionov, Y. Y. et al. Improved hysteresis and reliability of MoS2 transistors with high-quality CVD growth and Al2O3 encapsulation. IEEE Electron Device Lett. 38, 1763–1766 (2017).

    Article  Google Scholar 

  46. Dahanayaka, D. H. et al. Optically transparent Au111 substrates: flat gold nanoparticle platforms for high-resolution scanning tunneling microscopy. J. Am. Chem. Soc. 128, 6052–6053 (2006).

    Article  Google Scholar 

  47. Cui, X. Bridging homogeneous and heterogeneous catalysis by heterogeneous single-metal-site catalysts. Nat. Catal. 1, 385–397 (2018).

    Article  Google Scholar 

  48. Reguera, J. et al. Anisotropic metal nanoparticles for surface enhanced Raman scattering. Chem. Soc. Rev. 46, 3866–3885 (2017).

    Article  Google Scholar 

  49. Zhang, Y. et al. A single-crystalline native dielectric for two-dimensional semiconductors with an equivalent oxide thickness below 0.5 nm. Nat. Electron. 5, 643–649 (2022).

    Article  Google Scholar 

  50. Uchiyama, H. et al. A monolayer MoS2 FET with an EOT of 1.1 nm achieved by the direct formation of a high-κ Er2O3 insulator through thermal evaporation. Small 19, 2207394 (2023).

    Article  Google Scholar 

  51. Liu, K. et al. A wafer-scale van der Waals dielectric made from an inorganic molecular crystal film. Nat. Electron. 4, 906–913 (2021).

    Article  Google Scholar 

  52. Tang, J. et al. Low power flexible monolayer MoS2 integrated circuits. Nat. Commun. 14, 3633 (2023).

    Article  Google Scholar 

Download references

Acknowledgements

J.W. acknowledges financial support from the National Natural Science Foundation of China (grant no. 92064005)) and the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (grant no. SKL202211SIC). F.L. acknowledges financial support from National key research and development program of China (grant no. 2021YFA1601004).

Author information

Authors and Affiliations

Authors

Contributions

J.W. convinced the original ideas and supervised the whole project. L.Z. performed the CVD growth, characterization, device fabrication and electrical measurements under the assistance of Z. Liu, W.A., J.C. Z. Lv, B.W. and M.Y. The paper was written by J.W. and L.Z. with input from other authors. F.L. cosupervised the whole project and gave constructive suggestions. All authors contributed to the scientific discussions.

Corresponding author

Correspondence to Jinxiong Wu.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Electronics thanks Yanyu Jia and Yury Illarionov for their contribution to the peer review of this work.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Figs. 1–24 and Table 1.

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, L., Liu, Z., Ai, W. et al. Vertically grown metal nanosheets integrated with atomic-layer-deposited dielectrics for transistors with subnanometre capacitance-equivalent thicknesses. Nat Electron 7, 662–670 (2024). https://doi.org/10.1038/s41928-024-01202-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41928-024-01202-3

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing