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Hypotaxy of wafer-scale single-crystal transition metal dichalcogenides

Nature volume 638, pages 957–964 (2025)Cite this article

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Abstract

Two-dimensional (2D) semiconductors, particularly transition metal dichalcogenides (TMDs), are promising for advanced electronics beyond silicon1,2,3. Traditionally, TMDs are epitaxially grown on crystalline substrates by chemical vapour deposition. However, this approach requires post-growth transfer to target substrates, which makes controlling thickness and scalability difficult. Here we introduce a method called hypotaxy (‘hypo’ meaning downward and ‘taxy’ meaning arrangement), which enables wafer-scale single-crystal TMD growth directly on various substrates, including amorphous and lattice-mismatched substrates, while preserving crystalline alignment with an overlying 2D template. By sulfurizing or selenizing a pre-deposited metal film under graphene, aligned TMD nuclei form, coalescing into a single-crystal film as graphene is removed. This method achieves precise MoS2 thickness control from monolayer to hundreds of layers on diverse substrates, producing 4-inch single-crystal MoS2 with high thermal conductivity (about 120 W m−1 K−1) and mobility (around 87 cm2 V−1 s−1). Furthermore, nanopores created in graphene using oxygen plasma treatment allow MoS2 growth at a lower temperature of 400 °C, compatible with back-end-of-line processes. This hypotaxy approach extends to other TMDs, such as MoSe2, WS2 and WSe2, offering a solution to substrate limitations in conventional epitaxy and enabling wafer-scale TMDs for monolithic three-dimensional integration.

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Fig. 1: Growth mechanisms of epitaxy and hypotaxy.
Fig. 2: Step-by-step process of hypotaxial growth.
Fig. 3: Layer controllability in hypotaxial growth of MoS2.
Fig. 4: Hypotaxial growth of 4-inch single-crystal MoS2.
Fig. 5: Thermal and electrical properties of hypotaxially grown single-crystal MoS2.

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Acknowledgements

This work was supported by the National Research Foundation of Korea Grants funded by the Korean Government (2021R1A2C3014316 and RS-2024-00401234). G.-H.L. acknowledges the support from the Institute of Engineering Research, the Institute of Applied Physics and the Inter-University Semiconductor Research Center at the Seoul National University. We thank Y. J. Hong for naming this technology ‘hypotaxy’.

Author information

Authors and Affiliations

  1. Department of Materials Science and Engineering, Seoul National University, Seoul, Republic of Korea

    Donghoon Moon, Wonsik Lee, Jinwoo Kim, Jiwoo Kim, Yeonjoon Jung, Hyun-Young Choi, Won Seok Choi, Hangyel Kim, Ji-Hwan Baek, Changheon Kim, Jaewoong Joo, Hyun-Geun Oh, Jeong Woo Han, Hyejin Jang & Gwan-Hyoung Lee

  2. Research Institute for Advanced Materials (RIAM), Seoul National University, Seoul, South Korea

    Chaesung Lim, Hangyel Kim, Ji-Hwan Baek, Jeong Woo Han, Hyejin Jang & Gwan-Hyoung Lee

  3. Functional Composite Materials Research Center, Korea Institute of Science and Technology, Jeonbuk, Republic of Korea

    Changheon Kim, Sukang Bae & Jangyup Son

  4. Department of Physics, Sogang University, Seoul, Republic of Korea

    Hajung Jang & Hyeonsik Cheong

  5. Research Center for Electronic and Optical Materials, National Institute for Materials Science, Tsukuba, Japan

    Kenji Watanabe

  6. International Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan

    Takashi Taniguchi

  7. Department of JBNU-KIST Industry-Academia Convergence Research, Jeonbuk National University, Jeonju-si, Republic of Korea

    Sukang Bae & Jangyup Son

  8. Division of Nano and Information Technology, KIST School University of Science and Technology (UST), Seoul, Republic of Korea

    Jangyup Son

  9. Samsung Advanced Institute of Technology (SAIT), Samsung Electronics, Suwon, Republic of Korea

    Huije Ryu & Junyoung Kwon

Authors
  1. Donghoon Moon
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  2. Wonsik Lee
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  3. Chaesung Lim
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  4. Jinwoo Kim
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  7. Hyun-Young Choi
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  8. Won Seok Choi
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  9. Hangyel Kim
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  11. Changheon Kim
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  21. Hyeonsik Cheong
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  22. Jeong Woo Han
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Contributions

D.M. and G.-H.L. designed and conceived the project. W.L. and Hyejin Jang conducted thermal conductivity measurements. C.L. and J.W.H. performed DFT calculations. Jinwoo Kim performed TEM imaging. Jiwoo Kim, C.K., S.B., J.S., Y.J. and H.-G.O. prepared graphene and TMD samples. H.-Y.C., W.S.C., J.J., H.R. and J. Kwon fabricated devices and performed electrical measurements. Hajung Jang and H.C. performed the SHG measurements. K.W. and T.T. supplied boron nitride crystals. D.M. and G.-H.L. jointly analysed the data and wrote the paper together through discussion with H.K. and J.-H.B.

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Correspondence to Gwan-Hyoung Lee.

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Extended data figures and tables

Extended Data Fig. 1 Comparison of the MoS2 films grown by the conventional sulfurization and the hypotaxy through graphene.

a, Schematic of the MoS2 growth processes for conventional sulfurization and hypotaxy through graphene. The Mo film deposited on a SiO2 substrate by e-beam evaporation was partially covered by exfoliated 1L-Gr. For sulfurization, 20 sccm of H2S and 130 sccm of argon gas were supplied at 1000 °C for 2 h. The uncovered Mo film turns into randomly oriented MoS2 layers, while the graphene-covered Mo film transforms into a uniformly layered MoS2 structure through the formation of MoS2 nuclei that are crystallographically aligned with the top graphene layer. b,c, Raman spectra of conventionally sulfurized MoS2 (b) and hypotaxially grown MoS2 (c) before and after the sulfurization process. The cross-sectional STEM images in the insets shows the morphologies of two samples.

Extended Data Fig. 2 Hypotaxial growth of MoSe2, WS2, and WSe2.

a-c, HR-TEM images and corresponding SAED patterns (insets) of MoSe2 (a), WS2 (b), and WSe2 (c), indicating the applicability of the hypotaxial growth for a variety of TMDs.

Extended Data Fig. 3 Energetic stability of crystallographically aligned MoS2 nucleus with a graphene nanopore.

a, Optimized structure of hexagonal structure of MoS2 monolayer below graphene with nanopores. Black, sky blue, and yellow spheres are C, Mo, and S atoms, respectively. b, Relative energies as a function of the rotation of the MoS2 around the center of the MoS2 nuclei. The relative energies were calculated with reference to the energy of the 0 degree of MoS2. c, Standard deviation of bond lengths of six C-S bonds at the edge of graphene nanopore as a function of the rotation of the MoS2.

Extended Data Fig. 4 Effect of temperature and time on the hypotaxial growth of MoS2.

a, TEM images of graphene/Mo samples sulfurized at 600, 700, 800, and 900 °C for 30 and 120 min. Because of no formation of nanopores at 600 °C, the Mo film covered by graphene was not sulfurized even after 120 min. Meanwhile, the MoS2 was hypotaxially grown at 700–900 °C. However, graphene was partially removed at these temperatures. The TEM images were taken from the specific regions with no remaining graphene. b, Raman spectra of hypotaxially grown MoS2 at different sulfurization temperatures. As the sulfurization temperature increases, the \({\text{E}}_{2\text{g}}^{1}\) and A1g peaks of MoS2 becomes more pronounced, indicating higher crystallinity.

Extended Data Fig. 5 Low-temperature hypotaxial growth of MoS2.

a, TEM image of oxygen plasma-treated graphene for generation of nanopores. The nanopores are marked by red arrows. b, Cross-sectional STEM image of hypotaxially grown MoS2 at 400 °C through oxygen plasma-treated graphene. c, HR-TEM image and corresponding SAED pattern (inset) of the same sample.

Extended Data Fig. 6 Hypotaxial growth of MoS2 on various substrates.

a, Schematic process for hypotaxial growth of MoS2 at 400 °C on graphite, HfO2, and Au. b-d, HR-TEM images and corresponding FFT patterns (insets) of hypotaxially grown MoS2 on graphite (b), HfO2 (c), and Au (d), respectively. The 10 nm-thick HfO2 and 50 nm-thick Au film were deposited by atomic layer deposition (ALD) method and e-beam evaporation, respectively. Thanks to the unique characteristic of hypotaxy, the MoS2 can be grown regardless of the crystal structures of the substrates.

Extended Data Fig. 7 Asymmetry analyses in diffraction profiles of SAED patterns.

a, BF-TEM image of transferred 1L-MoS2 (hypotaxially grown at 1000 °C) onto a holey TEM grid. b, Representative SAED pattern of region 1. The diffraction intensity profile of spot 1 and 2 was extracted from the yellow dashed region. c, Diffraction intensity profiles obtained from twelve regions indicated in (a). These diffraction intensity profiles show that all regions have stronger intensity at spot 1 compared to spot 2, confirming these areas have the same crystalline orientation.

Extended Data Fig. 8 HR-TEM images of fifty regions with the same crystalline orientation and no twin boundaries.

HR-TEM images (10 nm × 10 nm) obtained from fifty regions of hypotaxially grown 1L-MoS2 at 1000 °C show no twin boundaries and all regions exhibit the same crystalline orientation. Regarding small distance between MoS2 nuclei (~10–20 nm), which correspond to the spacing between nanopores in graphene (Fig. 2f and Extended Data Fig. 6), absence of twin boundaries over this large area (fifty regions of 50 nm × 100 nm) strongly suggests that the hypotaxially grown MoS2 is a single crystal with no inversion domains.

Extended Data Fig. 9 Etching behavior of epitaxially and hypotaxially grown 1L-MoS2.

SEM images of a, epitaxially grown MoS2 on a c-sapphire substrate and b, hypotaxially grown MoS2 at 1000 °C after annealing at 1000 °C under low pressure of <10−3 Torr. The mild etching processes are widely used to visualize grain boundaries and determine crystalline orientation33,34,35,36. The SEM images were taken from different regions to investigate crystalline orientation of large area. The epitaxially grown 1L-MoS2 showed two triangular etched regions with opposite directions (indicated by red and yellow dashed lines) due to presence of grains with 0° and 60° orientations on the c-sapphire substrate as shown in (a). Meanwhile, the hypotaxially grown MoS2 exhibited unidirectional triangular shapes as shown in (b), indicating that the entire area etched by vacuum annealing is unidirectionally oriented.

Extended Data Fig. 10 Device performances of hypotaxial grown 1L-MoS2 with metal electrodes of Al/Cr/Au.

Transfer curves (Ids−Vgs) of back-gated hypotaxially grown 1L-MoS2 device with Al/Cr/Au contacts, showing high Ion/Ioff of > 109 and field-effect mobility of 79 cm2 V−1s−1. The linear output curves (Ids−Vds) in the inset show that the metal contacts are ohmic-like.

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Moon, D., Lee, W., Lim, C. et al. Hypotaxy of wafer-scale single-crystal transition metal dichalcogenides. Nature 638, 957–964 (2025). https://doi.org/10.1038/s41586-024-08492-9

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