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:

Oriented lateral growth of two-dimensional materials on c-plane sapphire

Nature Nanotechnology volume 18, pages 1289–1294 (2023)Cite this article

Subjects

Abstract

Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs) represent the ultimate thickness for scaling down channel materials. They provide a tantalizing solution to push the limit of semiconductor technology nodes in the sub-1 nm range. One key challenge with 2D semiconducting TMD channel materials is to achieve large-scale batch growth on insulating substrates of single crystals with spatial homogeneity and compelling electrical properties. Recent studies have claimed the epitaxy growth of wafer-scale, single-crystal 2D TMDs on a c-plane sapphire substrate with deliberately engineered off-cut angles. It has been postulated that exposed step edges break the energy degeneracy of nucleation and thus drive the seamless stitching of mono-oriented flakes. Here we show that a more dominant factor should be considered: in particular, the interaction of 2D TMD grains with the exposed oxygen–aluminium atomic plane establishes an energy-minimized 2D TMD–sapphire configuration. Reconstructing the surfaces of c-plane sapphire substrates to only a single type of atomic plane (plane symmetry) already guarantees the single-crystal epitaxy of monolayer TMDs without the aid of step edges. Electrical results evidence the structural uniformity of the monolayers. Our findings elucidate a long-standing question that curbs the wafer-scale batch epitaxy of 2D TMD single crystals—an important step towards using 2D materials for future electronics. Experiments extended to perovskite materials also support the argument that the interaction with sapphire atomic surfaces is more dominant than step-edge docking.

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

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

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

Fig. 1: Computer-generated atomic structure of a c-plane sapphire (α-Al2O3) and the associated DFT calculations of absorption energy of MoS2 at various rotation angles.
Fig. 2: Stark contrasts in nucleating MoS2 seeds on c-plane sapphire terraces with alternating and identical exposing surfaces.
Fig. 3: Wafer-scale monolayer MoS2 films with continuous single crystallinity on c-plane sapphire.
Fig. 4: Batch fabrication of monolayer MoS2 FETs.

Similar content being viewed by others

Data availability

The data from this study are available from the corresponding authors on reasonable request.

References

  1. Liu, C. et al. 2D materials-based static random-access memory. Adv. Mater. 34, 2107894 (2022).

    Article  CAS  Google Scholar 

  2. Wan, Y. et al. Wafer-scale single-orientation 2D layers by atomic edge-guided epitaxial growth. Chem. Soc. Rev. 51, 803–811 (2022).

    Article  CAS  Google Scholar 

  3. Chubarov, M. et al. Wafer-scale epitaxial growth of unidirectional WS2 monolayers on sapphire. ACS Nano 15, 2532–2541 (2021).

    Article  CAS  Google Scholar 

  4. Li, T. et al. Epitaxial growth of wafer-scale molybdenum disulfide semiconductor single crystals on sapphire. Nat. Nanotechnol. 16, 1201–1207 (2021).

    Article  CAS  Google Scholar 

  5. Vlassiouk, I. V. et al. Evolutionary selection growth of two-dimensional materials on polycrystalline substrates. Nat. Mater. 17, 318–322 (2018).

    Article  CAS  Google Scholar 

  6. Zhang, B. Y. et al. Hexagonal metal oxide monolayers derived from the metal–gas interface. Nat. Mater. 20, 1073–1078 (2021).

    Article  CAS  Google Scholar 

  7. Tusche, C., Meyerheim, H. L. & Kirschner, J. Observation of depolarized ZnO(0001) monolayers: formation of unreconstructed planar sheets. Phys. Rev. Lett. 99, 026102 (2007).

    Article  CAS  Google Scholar 

  8. Dong, J., Zhang, L., Dai, X. & Ding, F. The epitaxy of 2D materials growth. Nat. Commun. 11, 5862 (2020).

    Article  CAS  Google Scholar 

  9. Devulapalli, V., Bishara, H., Ghidelli, M., Dehm, G. & Liebscher, C. H. Influence of substrates and e-beam evaporation parameters on the microstructure of nanocrystalline and epitaxially grown Ti thin films. Appl. Surf. Sci. 562, 150194 (2021).

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  11. 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  CAS  Google Scholar 

  12. Yang, P. et al. Epitaxial growth of centimeter-scale single-crystal MoS2 monolayer on Au(111). ACS Nano 14, 5036–5045 (2020).

    Article  CAS  Google Scholar 

  13. Dumcenco, D. et al. Large-area epitaxial monolayer MoS2. ACS Nano 9, 4611–4620 (2015).

    Article  CAS  Google Scholar 

  14. Yu, H. et al. Wafer-scale growth and transfer of highly-oriented monolayer MoS2 continuous films. ACS Nano 11, 12001–12007 (2017).

    Article  CAS  Google Scholar 

  15. Aljarb, A. et al. Substrate lattice-guided seed formation controls the orientation of 2D transition-metal dichalcogenides. ACS Nano 11, 9215–9222 (2017).

    Article  CAS  Google Scholar 

  16. Suenaga, K. et al. Surface-mediated aligned growth of monolayer MoS2 and in-plane heterostructures with graphene on sapphire. ACS Nano 12, 10032–10044 (2018).

    Article  CAS  Google Scholar 

  17. Zhang, X. et al. Diffusion-controlled epitaxy of large area coalesced WSe2 monolayers on sapphire. Nano Lett. 18, 1049–1056 (2018).

    Article  CAS  Google Scholar 

  18. Wang, Q. et al. Wafer-scale highly oriented monolayer MoS2 with large domain sizes. Nano Lett. 20, 7193–7199 (2020).

    Article  CAS  Google Scholar 

  19. Toofan, J. & Watson, P. R. The termination of the α-Al2O3 (0001) surface: a LEED crystallography determination. Surf. Sci. 401, 162–172 (1998).

    Article  CAS  Google Scholar 

  20. Chiang, Y.-M., Birnie, D. P. & Kingery, W. D. Physical Ceramics: Principles for Ceramic Science and Engineering (John Wiley & Sons, 1997).

  21. Ji, Q. et al. Unravelling orientation distribution and merging behavior of monolayer MoS2 domains on sapphire. Nano Lett. 15, 198–205 (2015).

    Article  CAS  Google Scholar 

  22. Yoshimoto, M. et al. Atomic‐scale formation of ultrasmooth surfaces on sapphire substrates for high‐quality thin‐film fabrication. Appl. Phys. Lett. 67, 2615–2617 (1995).

    Article  CAS  Google Scholar 

  23. Pham Van, L., Kurnosikov, O. & Cousty, J. Evolution of steps on vicinal (0001) surfaces of α-alumina. Surf. Sci. 411, 263–271 (1998).

    Article  CAS  Google Scholar 

  24. Thune, E., Fakih, A., Matringe, C., Babonneau, D. & Guinebretière, R. Understanding of one dimensional ordering mechanisms at the (001) sapphire vicinal surface. J. Appl. Phys. 121, 015301 (2017).

    Article  Google Scholar 

  25. Koma, A. Van der Waals epitaxy for highly lattice-mismatched systems. J. Cryst. Growth 201–202, 236–241 (1999).

    Article  Google Scholar 

  26. Lin, Y.-C. et al. Realizing large-scale, electronic-grade two-dimensional semiconductors. ACS Nano 12, 965–975 (2018).

    Article  CAS  Google Scholar 

  27. Shi, Y. et al. Engineering wafer-scale epitaxial two-dimensional materials through sapphire template screening for advanced high-performance nanoelectronics. ACS Nano 15, 9482–9494 (2021).

    Article  CAS  Google Scholar 

  28. Chen, L. et al. Step-edge-guided nucleation and growth of aligned WSe2 on sapphire via a layer-over-layer growth mode. ACS Nano 9, 8368–8375 (2015).

    Article  CAS  Google Scholar 

  29. Fang, F. et al. Two-dimensional Cs2AgBiBr6/WS2 heterostructure-based photodetector with boosted detectivity via interfacial engineering. ACS Nano 16, 3985–3993 (2022).

    Article  CAS  Google Scholar 

  30. Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169–11186 (1996).

    Article  CAS  Google Scholar 

  31. Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).

    Article  CAS  Google Scholar 

  32. Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953–17979 (1994).

    Article  Google Scholar 

  33. Grimme, S., Antony, J., Ehrlich, S. & Krieg, H. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J. Chem. Phys. 132, 154104 (2010).

    Article  Google Scholar 

Download references

Acknowledgements

J.-H.F. and V.T. are indebted to the financial support from the University of Tokyo and the Japan Society for the Promotion of Science (JSPS, 23H00253). V.T. is beholden to the support from the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under award CCF-3079 and Office of Technology Development under the RTF grant. L.-J.L. acknowledges support from the Jockey Club Hong Kong to the JC STEM lab of 3DIC and the Research Grant of the Council of Hong Kong (CRS_PolyU502/22). Y.W. and L.-J.L. acknowledge support from the University of Hong Kong and the National Key R&D Project of China (2022YFB4044100). J.-H.F. and V.T. acknowledge KAUST Core Labs and the National Synchrotron Radiation Research Center (NSRRC) for support for the STEM imaging and LEED characterization. Y.-J.L. acknowledges support from AS-CDA-108-M08 Academia Sinica. J.-H.F. and V.T. dedicate this work to Ibrahim Alnami, who passed away before completing this project.

Author information

Author notes

  1. Deceased: I. Alnami.

Authors and Affiliations

  1. Department of Chemical System Engineering, School of Engineering, The University of Tokyo, Tokyo, Japan

    Jui-Han Fu, Chien-Chih Tseng, Hayato Sugisaki & Vincent Tung

  2. Department of Civil Engineering, The University of Hong Kong, Hong Kong, China

    Jiacheng Min & Kaimin Shih

  3. Department of Electrophysics, National Yang-Ming Chiao Tung University, Hsinchu, Taiwan

    Che-Kang Chang, Tzu-Hsuan Lo, Zih-Siang Jian & Wen-Hao Chang

  4. Physical Sciences and Engineering Division, King Abdullah University of Science and Technology (KAUST), Thuwal, Saudi Arabia

    Chien-Chih Tseng, Qingxiao Wang & Ibrahim Alnami

  5. Department of Mechanical Engineering, The University of Hong Kong, Hong Kong, China

    Chenyang Li, Yu-Ming Chang, Ci Lin, Lain-Jong Li & Yi Wan

  6. Research Centre for Applied Sciences, Academia Sinica, Taipei, Taiwan

    Wei-Ren Syong, Wen-Hao Chang & Yu-Jung Lu

  7. College of Electronics and Information Engineering, Shenzhen University, Shenzhen, China

    Feier Fang, Lv Zhao & Yumeng Shi

  8. Department of Electronic Engineering, Chang Gung University, Taoyuan, Taiwan

    Chao-Sung Lai

  9. National Synchrotron Radiation Research Center, Hsinchu, Taiwan

    Wei-Sheng Chiu

  10. Center for Green Technology of the Chang Gung University, Taoyuan, Taiwan

    Vincent Tung

Authors
  1. Jui-Han Fu
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Jiacheng Min
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Che-Kang Chang
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Chien-Chih Tseng
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Qingxiao Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Hayato Sugisaki
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Chenyang Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Yu-Ming Chang
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Ibrahim Alnami
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Wei-Ren Syong
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Ci Lin
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Feier Fang
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. Lv Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  14. Tzu-Hsuan Lo
    View author publications

    You can also search for this author in PubMed Google Scholar

  15. Chao-Sung Lai
    View author publications

    You can also search for this author in PubMed Google Scholar

  16. Wei-Sheng Chiu
    View author publications

    You can also search for this author in PubMed Google Scholar

  17. Zih-Siang Jian
    View author publications

    You can also search for this author in PubMed Google Scholar

  18. Wen-Hao Chang
    View author publications

    You can also search for this author in PubMed Google Scholar

  19. Yu-Jung Lu
    View author publications

    You can also search for this author in PubMed Google Scholar

  20. Kaimin Shih
    View author publications

    You can also search for this author in PubMed Google Scholar

  21. Lain-Jong Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  22. Yi Wan
    View author publications

    You can also search for this author in PubMed Google Scholar

  23. Yumeng Shi
    View author publications

    You can also search for this author in PubMed Google Scholar

  24. Vincent Tung
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

J.-H.F., L.-J.L. and V.T. conceived the project. J.-H.F. and H.S. restructured the c-plane sapphire and accomplished the AFM and cross-sectional STEM characterizations. J.-H.F., C.-K.C., Y.-M.C., C. Li, T.-H.L., Z.-S.J., I.A. and C.-C.T. synthesized the TMDs and carried out the Raman and photoluminescence characterizations. J.M., Y.W. and K.S. performed the first-principles calculations. C. Lin, C.-K.C., W.-H.C. and J.-H.F. executed the SHG analysis and LEED analysis. C.-K.C., W.-R.S., C.-S.L. and Y.-J.L. accomplished the fabrication and electrical characterization of MoS2 FETs. F.F., L.Z. and Y.S. synthesized and characterized the Cs2AgBiBr6 crystals. Q.W. conducted HRTEM and image analysis. W.-S.C. carried out LEED analysis. All the authors discussed and contributed to the results. J.-H.F., Y.W., L.-J.L. and V.T. wrote the paper.

Corresponding authors

Correspondence to Lain-Jong Li, Yi Wan, Yumeng Shi or Vincent Tung.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Nanotechnology thanks Kibum Kang and the other, anonymous, reviewer(s) 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. 1–12.

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

Fu, JH., Min, J., Chang, CK. et al. Oriented lateral growth of two-dimensional materials on c-plane sapphire. Nat. Nanotechnol. 18, 1289–1294 (2023). https://doi.org/10.1038/s41565-023-01445-9

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41565-023-01445-9

This article is cited by

Search

Advanced 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