Letter | Published:

High-mobility three-atom-thick semiconducting films with wafer-scale homogeneity

Nature volume 520, pages 656660 (30 April 2015) | Download Citation

Abstract

The large-scale growth of semiconducting thin films forms the basis of modern electronics and optoelectronics. A decrease in film thickness to the ultimate limit of the atomic, sub-nanometre length scale, a difficult limit for traditional semiconductors (such as Si and GaAs), would bring wide benefits for applications in ultrathin and flexible electronics, photovoltaics and display technology1,2,3. For this, transition-metal dichalcogenides (TMDs), which can form stable three-atom-thick monolayers4, provide ideal semiconducting materials with high electrical carrier mobility5,6,7,8,9,10, and their large-scale growth on insulating substrates would enable the batch fabrication of atomically thin high-performance transistors and photodetectors on a technologically relevant scale without film transfer. In addition, their unique electronic band structures provide novel ways of enhancing the functionalities of such devices, including the large excitonic effect11, bandgap modulation12, indirect-to-direct bandgap transition13, piezoelectricity14 and valleytronics15. However, the large-scale growth of monolayer TMD films with spatial homogeneity and high electrical performance remains an unsolved challenge. Here we report the preparation of high-mobility 4-inch wafer-scale films of monolayer molybdenum disulphide (MoS2) and tungsten disulphide, grown directly on insulating SiO2 substrates, with excellent spatial homogeneity over the entire films. They are grown with a newly developed, metal–organic chemical vapour deposition technique, and show high electrical performance, including an electron mobility of 30 cm2 V−1 s−1 at room temperature and 114 cm2 V−1 s−1 at 90 K for MoS2, with little dependence on position or channel length. With the use of these films we successfully demonstrate the wafer-scale batch fabrication of high-performance monolayer MoS2 field-effect transistors with a 99% device yield and the multi-level fabrication of vertically stacked transistor devices for three-dimensional circuitry. Our work is a step towards the realization of atomically thin integrated circuitry.

Access optionsAccess options

Rent or Buy article

Get time limited or full article access on ReadCube.

from$8.99

All prices are NET prices.

References

  1. 1.

    , & Materials and mechanics for stretchable electronics. Science 327, 1603–1607 (2010).

  2. 2.

    et al. Ultrathin compound semiconductor on insulator layers for high-performance nanoscale transistors. Nature 468, 286–289 (2010).

  3. 3.

    , , , & High-mobility ultrathin semiconducting films prepared by spin coating. Nature 428, 299–303 (2003).

  4. 4.

    & Van der Waals heterostructures. Nature 499, 419–425 (2013).

  5. 5.

    , & Phonon-limited mobility in n-type single-layer MoS2 from first principles. Phys. Rev. B 85, 115317 (2012).

  6. 6.

    , , & Intrinsic electronic transport properties of high-quality monolayer and bilayer MoS2. Nano Lett. 13, 4212–4216 (2013).

  7. 7.

    & Mobility engineering and a metal–insulator transition in monolayer MoS2. Nature Mater. 12, 815–820 (2013).

  8. 8.

    et al. Transport properties of monolayer MoS2 grown by chemical vapor deposition. Nano Lett. 14, 1909–1913 (2014).

  9. 9.

    et al. Band-like transport in high mobility unencapsulated single-layer MoS2 transistors. Appl. Phys. Lett. 102, 173107 (2013).

  10. 10.

    et al. Electrical transport properties of single-layer WS2. ACS Nano 8, 8174–8181 (2014).

  11. 11.

    et al. Probing excitonic dark states in single-layer tungsten disulphide. Nature 513, 214–218 (2014).

  12. 12.

    et al. Growth of large-area 2D MoS2(1−x)Se2x semiconductor alloys. Adv. Mater. 26, 2648–2653 (2014).

  13. 13.

    , , , & Atomically thin MoS2: a new direct-gap semiconductor. Phys. Rev. Lett. 105, 136805 (2010).

  14. 14.

    et al. Piezoelectricity of single-atomic-layer MoS2 for energy conversion and piezotronics. Nature 514, 470–474 (2014).

  15. 15.

    , , & The valley Hall effect in MoS2 transistors. Science 344, 1489–1492 (2014).

  16. 16.

    et al. Wafer-scale MoS2 thin layers prepared by MoO3 sulfurization. Nanoscale 4, 6637–6641 (2012).

  17. 17.

    et al. Patternable large-scale molybdenium disulfide atomic layers grown by gold-assisted chemical vapor deposition. Angew. Chem. Int. Ed. 53, 1266–1269 (2014).

  18. 18.

    et al. Vapour phase growth and grain boundary structure of molybdenum disulphide atomic layers. Nature Mater. 12, 754–759 (2013).

  19. 19.

    et al. Grains and grain boundaries in highly crystalline monolayer molybdenum disulphide. Nature Mater. 12, 554–561 (2013).

  20. 20.

    et al. Synthesis and transfer of single-layer transition metal disulfides on diverse surfaces. Nano Lett. 13, 1852–1857 (2013).

  21. 21.

    et al. Statistical study of deep submicron dual-gated field-effect transistors on monolayer chemical vapor deposition molybdenum disulfide films. Nano Lett. 13, 2640–2646 (2013).

  22. 22.

    et al. Controlled scalable synthesis of uniform, high-quality monolayer and few-layer MoS2 films. Sci. Rep. 3, 1866 (2013).

  23. 23.

    et al. Controlled growth of high-quality monolayer WS2 layers on sapphire. ACS Nano 7, 8963–8971 (2013).

  24. 24.

    et al. Evolution of electronic structure in atomically thin sheets of WS2 and WSe2. ACS Nano 7, 791–797 (2013).

  25. 25.

    et al. From bulk to monolayer MoS2: evolution of Raman scattering. Adv. Funct. Mater. 22, 1385–1390 (2012).

  26. 26.

    et al. Identification of individual and few layers of WS2 using Raman spectroscopy. Sci. Rep. 3, 1755 (2013).

  27. 27.

    & Growth and Properties of Ultrathin Epitaxial Layers (Elsevier, 1997).

  28. 28.

    & Hydrogenolysis of oxygenated organic compounds. J. Am. Chem. Soc. 54, 4678–4690 (1932).

  29. 29.

    et al. Theoretical study of the MoS2 (100) surface: a chemical potential analysis of sulfur and hydrogen coverage. J. Phys. Chem. B 104, 11220–11229 (2000).

  30. 30.

    et al. Electrical transport properties of polycrystalline monolayer molybdenum disulfide. ACS Nano 8, 7930–7937 (2014).

Download references

Acknowledgements

We thank P. L. McEuen, M.-H. Jo, H. Heo and H.-C. Choi for discussions, and M. Guimaraes and Z. Ziegler for help in preparing the manuscript. This work was supported mainly by the AFOSR (FA2386-13-1-4118 and FA9550-11-1-0033) and the Nano Material Technology Development Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT, and Future Planning (2012M3A7B4049887). Additional funding was provided by the National Science Foundation (NSF) through the Cornell Center for Materials Research (NSF DMR-1120296) and by the Samsung Advanced Institute for Technology GRO Program. Device fabrication was performed at the Cornell NanoScale Facility, a member of the National Nanotechnology Infrastructure Network, which is supported by the National Science Foundation (ECS-0335765).

Author information

Author notes

    • Kibum Kang
    •  & Saien Xie

    These authors contributed equally to this work.

Affiliations

  1. Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853, USA

    • Kibum Kang
    • , Lujie Huang
    • , Cheol-Joo Kim
    •  & Jiwoong Park
  2. School of Applied and Engineering Physics, Cornell University, Ithaca, New York 14853, USA

    • Saien Xie
    • , Yimo Han
    • , Pinshane Y. Huang
    •  & David Muller
  3. Kavli Institute at Cornell for Nanoscale Science, Ithaca, New York 14853, USA

    • Kin Fai Mak
    • , David Muller
    •  & Jiwoong Park
  4. Laboratory of Atomic and Solid State Physics, Cornell University, Ithaca, New York 14853, USA

    • Kin Fai Mak

Authors

  1. Search for Kibum Kang in:

  2. Search for Saien Xie in:

  3. Search for Lujie Huang in:

  4. Search for Yimo Han in:

  5. Search for Pinshane Y. Huang in:

  6. Search for Kin Fai Mak in:

  7. Search for Cheol-Joo Kim in:

  8. Search for David Muller in:

  9. Search for Jiwoong Park in:

Contributions

K.K. and S.X. contributed equally to this work. K.K, S.X. and J.P. conceived the experiments. K.K. and S.X. performed the synthesis, optical characterization, device fabrication, and electrical measurements. L.H. conducted low-temperature electrical measurement, with assistance from K.F.M. Y.H, P.Y.H. and D.A.M. performed atomic resolution STEM imaging. K.K. carried out DF-TEM and data analysis, with assistance from C.-J.K. K.K, S.X. and J.P. wrote the manuscript. All authors discussed the results and commented on the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Jiwoong Park.

Supplementary information

PDF files

  1. 1.

    Supplementary Information

    This file contains Supplementary Methods, Supplementary Notes, Supplementary Figures 1-17 and additional references.

About this article

Publication history

Received

Accepted

Published

DOI

https://doi.org/10.1038/nature14417

Further reading

Comments

By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.