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Heteroepitaxial van der Waals semiconductor superlattices

Nature Nanotechnology volume 16, pages 1092–1098 (2021)Cite this article

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Abstract

A broad range of transition metal dichalcogenide (TMDC) semiconductors are available as monolayer (ML) crystals, so the precise integration of each kind into van der Waals (vdW) superlattices (SLs) could enable the realization of novel structures with previously unexplored functionalities. Here we report the atomic layer-by-layer epitaxial growth of vdW SLs with programmable stacking periodicities, composed of more than two kinds of dissimilar TMDC MLs, such as MoS2, WS2 and WSe2. Using kinetics-controlled vdW epitaxy in the near-equilibrium limit by metal–organic chemical vapour depositions, we achieved precise ML-by-ML stacking, free of interlayer atomic mixing, which resulted in tunable two-dimensional vdW electronic systems. As an example, by exploiting the series of type II band alignments at coherent two-dimensional vdW heterointerfaces, we demonstrated valley-polarized carrier excitations—one of the most distinctive electronic features in vdW ML semiconductors—which scale with the stack numbers n in our (MoS2/WS2)n SLs on optical excitations.

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Fig. 1: ML-by-ML vdW heteroepitaxy of MoS2/WS2 SLs.
Fig. 2: Designer heteroepitaxy of vdW SLs with tunable periodicities.
Fig. 3: Heteroepitaxial evolution of in-plane crystalline textures of WSe2/WS2/MoS2 trilayers.
Fig. 4: Valley-polarized interlayer excitations in the type II MoS2/WS2 SLs.

Data availability

Presented measurement data within this article and other findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This work was supported by the Institute for Basic Science (IBS), Korea, under Project Code IBS-R014-A1.

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Author notes

  1. These authors contributed equally: Gangtae Jin, Chang-Soo Lee.

Authors and Affiliations

  1. Center for Artificial Low Dimensional Electronic Systems, Institute for Basic Science (IBS), Pohang, Korea

    Gangtae Jin, Chang-Soo Lee, Suk-Ho Lee, Min Yeong Park, Soonyoung Cha, Seung-Young Seo, Gunho Moon, Seok Young Min, Cheolhee Han, Jonghwan Kim & Moon-Ho Jo

  2. Department of Materials Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, Korea

    Gangtae Jin, Chang-Soo Lee, Odongo F. N. Okello, Suk-Ho Lee, Min Yeong Park, Seung-Young Seo, Gunho Moon, Seok Young Min, Dong-Hwan Yang, Cheolhee Han, Jonghwan Kim, Si-Young Choi & Moon-Ho Jo

  3. Pohang Accelerator Laboratory, Pohang, Korea

    Hyungju Ahn

  4. Department of Physics & Astronomy, Seoul National University, Seoul, Korea

    Jekwan Lee & Hyunyong Choi

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Contributions

G.J., C.-S.L. and M.-H.J. conceived and designed the project. G.J., C.-S.L., S.-H.L. and M.Y.P. conducted the MOCVD growth experiments and material characterizations. O.F.N.O., D.-H.Y. and S.-Y.C. performed the TEM measurements and analysed the data. S.-Y.S., G.M. and S.Y.M. fabricated the devices and performed the optical measurements. H.A. performed the GI-WAXD measurements. S.C., C.H., J.L., J.K. and H.C. carried out the ultrafast laser spectroscopy. G.J., C.-S.L., S.C. and M.-H.J. wrote the paper. M.-H.J. supervised the project. All the authors discussed the results and commented on the manuscript.

Corresponding author

Correspondence to Moon-Ho Jo.

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Peer review information Nature Nanotechnology thanks Kian Ping Loh, Anlian Pan and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Note, Figs. 1–29, Tables 1–3 and references 1–12.

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Jin, G., Lee, CS., Okello, O.F.N. et al. Heteroepitaxial van der Waals semiconductor superlattices. Nat. Nanotechnol. 16, 1092–1098 (2021). https://doi.org/10.1038/s41565-021-00942-z

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