Abstract
Twisted van der Waals heterostructures (vdWHs) designed with atomic-scale precision have interesting properties and are important for modern electronics. However, fabricating large-area, two-dimensional (2D) vdWHs with clean interfaces and controllable twist angles remains challenging. Here we successfully fabricated twisted graphene (Gr)/hexagonal boron nitride (h-BN) heterojunctions under vacuum by developing a quasi-melting transfer technique for Gr/Ge (110) and h-BN/Ge (210) substrates. By precisely aligning the Gr/Ge and h-BN/Ge stacks with specific in-plane lattices, we achieved ultraclean transfer of Gr/h-BN superlattices with adjustable stacking orders and precise angles through the sequential transfer of Gr and h-BN monolayers. Transmission electron microscopy, atomic force microscopy, nano angle-resolved photoemission spectroscopy and second-harmonic generation measurement confirmed that the Gr/h-BN superlattices fabricated exhibit atomic-level precision, are of high quality, are free of wrinkles and have controllable twist angles. Theoretical calculations demonstrated that breaking the Ge–Ge bonds in the melted substrate greatly weakens the binding strength of Gr and h-BN to the surface, thereby facilitating the clean transfer of the 2D materials. This study provides a viable pathway for the precise fabrication of large-scale 2D vdWHs and lays a solid material foundation for their application in next-generation electronic devices.
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The data supporting the findings of this study are provided in Supplementary Information. Source data are provided with this paper.
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Acknowledgements
We are grateful to X. Yue and C. Cong from Fudan University for Raman mapping characterization. We are grateful to B. Yang and J. Liu from Shanghai Tech University for DFT calculations. T.W. and W.G. acknowledge support from the National Key Research and Development Project of China (grant nos 2024YFA1410600 and 2021YFA1200801), the National Natural Science Foundation of China (grant nos 62174169, 12104476 and 22173031) and the Key Project of Frontier Science Research of Chinese Academy of Sciences (grant no. XDB30000000). C.Z. acknowledges support from National Natural Science Foundation of China (grant no. 52402195) and the China Postdoctoral Science Foundation (grant no. 2023M742225). H.W. acknowledges support from National Natural Science Foundation of China (grant nos 91964102, 51772317, 12004406, 62074099 and 12304113).
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C.Z. and Q.X. contributed equally to this work. T.W. and C.Z. conceived the project. C.Z. and B.G. performed the growth and transfer experiments. C. Jiang and H.W. performed the AFM measurements. B.W. and C. Jin performed the TEM and SAED experiments. W.G., J.W., C.Z. and K.Y. performed the EELS experiments. Q.Y. and Q.X. performed the calculations. Z.C. conducted the SHG characterizations. H.X. and Z.L. conducted the ARPES characterizations. W.G., Q.Y., T.W. and T.D. provided comprehensive guidance and financial support for all experiments and characterization. All the authors revised and commented on the paper.
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Nature Synthesis thanks Peter Bøggild, Miguel Espitia-Rico and Libo Gao for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team.
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Zhang, C., Xie, Q., Jiang, C. et al. Melting-assisted assembly of twisted graphene/h-BN superlattices with clean interfaces. Nat. Synth (2026). https://doi.org/10.1038/s44160-026-01000-z
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DOI: https://doi.org/10.1038/s44160-026-01000-z
