Abstract
Two-dimensional (2D) materials, such as graphene, transition metal dichalcogenides (TMDs) and hexagonal boron nitride, exhibit intriguing properties that are sensitive to their atomic-scale structures and can be further enriched through van der Waals (vdW) integration. However, the precise synthesis and clean integration of 2D materials remain challenging. Here, using graphene or hexagonal boron nitride as a vdW capping layer, we create a nano-confined environment that directs the growth kinetics of 2D TMDs (such as NbSe2 and MoS2), enabling precise formation of TMD monolayers with tailored morphologies, from isolated monolayer domains to large-scale continuous films and intrinsically patterned rings. Moreover, Janus S–Mo–Se monolayers are synthesized with atomic precision via vdW-protected bottom-plane chalcogen substitution. Importantly, our approach simultaneously produces ultraclean vdW interfaces. This in situ encapsulation reliably preserves air-sensitive materials, as evidenced by the enhanced superconductivity of nano-confined NbSe2 monolayers. Altogether, our study establishes a versatile platform for the controlled synthesis and integration of 2D TMDs for advanced applications.
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References
Zou, X. et al. Robust epitaxy of single-crystal transition-metal dichalcogenides on lanthanum-passivated sapphire. Science 390, eaea0849 (2025).
Moon, D. et al. Hypotaxy of wafer-scale single-crystal transition metal dichalcogenides. Nature 638, 957–964 (2025).
Zhou, Z. et al. Stack growth of wafer-scale van der Waals superconductor heterostructures. Nature 621, 499–505 (2023).
Liu, L. et al. Uniform nucleation and epitaxy of bilayer molybdenum disulfide on sapphire. Nature 605, 69–75 (2022).
Li, J. et al. General synthesis of two-dimensional van der Waals heterostructure arrays. Nature 579, 368–374 (2020).
Park, H. et al. Observation of fractionally quantized anomalous Hall effect. Nature 622, 74–79 (2023).
Lin, J.-X. et al. Spin–orbit-driven ferromagnetism at half moiré filling in magic-angle twisted bilayer graphene. Science 375, 437–441 (2022).
Weston, A. et al. Interfacial ferroelectricity in marginally twisted 2D semiconductors. Nat. Nanotechnol. 17, 390–395 (2022).
Wang, L. et al. Correlated electronic phases in twisted bilayer transition metal dichalcogenides. Nat. Mater. 19, 861–866 (2020).
Zai, H. et al. Wafer-scale monolayer MoS2 film integration for stable, efficient perovskite solar cells. Science 387, 186–192 (2025).
Mennel, L. et al. Ultrafast machine vision with 2D material neural network image sensors. Nature 579, 62–66 (2020).
He, Y. et al. Amorphizing noble metal chalcogenide catalysts at the single-layer limit towards hydrogen production. Nat. Catal. 5, 212–221 (2022).
Cappelluti, E., Roldán, R., Silva-Guillén, J. A., Ordejón, P. & Guinea, F. Tight-binding model and direct-gap/indirect-gap transition in single-layer and multilayer MoS2. Phys. Rev. B 88, 075409 (2013).
Xi, X. et al. Ising pairing in superconducting NbSe2 atomic layers. Nat. Phys. 12, 139–143 (2015).
Lu, A.-Y. et al. Janus monolayers of transition metal dichalcogenides. Nat. Nanotechnol. 12, 744–749 (2017).
Zhang, J. et al. Janus monolayer transition-metal dichalcogenides. ACS Nano 11, 8192–8198 (2017).
Lin, Y.-C. et al. Low energy implantation into transition-metal dichalcogenide monolayers to form Janus structures. ACS Nano 14, 3896–3906 (2020).
Trivedi, D. B. et al. Room-temperature synthesis of 2D Janus crystals and their heterostructures. Adv. Mater. 32, 2006320 (2020).
Guo, Y. et al. Designing artificial two-dimensional landscapes via atomic substitution. Proc. Natl Acad. Sci. USA 118, e2106124118 (2021).
Gan, Z. et al. Chemical vapor deposition of high-optical-quality large-area monolayer Janus transition metal dichalcogenides. Adv. Mater. 34, 2205226 (2022).
Dong, L., Lou, J. & Shenoy, V. B. Large in-plane and vertical piezoelectricity in Janus transition metal dichalchogenides. ACS Nano 11, 8242–8248 (2017).
Patel, A., Singh, D., Sonvane, Y., Thakor, P. B. & Ahuja, R. High thermoelectric performance in two-dimensional Janus monolayer material WS-X (X = Se and Te). ACS Appl. Mater. Interfaces 12, 46212–46219 (2020).
Liu, J. & Pantelides, S. T. Mechanisms of pyroelectricity in three- and two-dimensional materials. Phys. Rev. Lett. 120, 207602 (2018).
Kang, K. et al. High-mobility three-atom-thick semiconducting films with wafer-scale homogeneity. Nature 520, 656–660 (2015).
Seol, M. et al. High-throughput growth of wafer-scale monolayer transition metal dichalcogenide via vertical Ostwald ripening. Adv. Mater. 32, 2003542 (2020).
Haigh, S. J. et al. Cross-sectional imaging of individual layers and buried interfaces of graphene-based heterostructures and superlattices. Nat. Mater. 11, 764–767 (2012).
Wang, H. et al. High-quality monolayer superconductor NbSe2 grown by chemical vapour deposition. Nat. Commun. 8, 394 (2017).
Zou, Y.-C. et al. Superconductivity and magnetotransport of single-crystalline NbSe2 nanoplates grown by chemical vapour deposition. Nanoscale 9, 16591–16595 (2017).
Park, S. et al. Tailoring Domain Morphology in Monolayer NbSe2 and WxNb1–xSe2 Heterostructure. ACS Nano 14, 8784–8792 (2020).
Hill, H. M. et al. Comprehensive optical characterization of atomically thin NbSe2. Phys. Rev. B 98, 165109 (2018).
Cao, Y. et al. Quality heterostructures from two-dimensional crystals unstable in air by their assembly in inert atmosphere. Nano Lett. 15, 4914–4921 (2015).
Telford, E. J. et al. Via method for lithography free contact and preservation of 2D materials. Nano Lett. 18, 1416–1420 (2018).
Rudenko, A. N., Keil, F. J., Katsnelson, M. I. & Lichtenstein, A. I. Interfacial interactions between local defects in amorphous SiO2 and supported graphene. Phys. Rev. B 84, 085438 (2011).
Li, J. et al. Wafer-scale single-crystal monolayer graphene grown on sapphire substrate. Nat. Mater. 21, 740–747 (2022).
Xiao, R.-F., Alexander, J. I. D. & Rosenberger, F. Growth morphology with anisotropic surface kinetics. J. Crystal Growth 100, 313–329 (1990).
Michely, T. & Krug, J. Islands, Mounds, and Atoms: Patterns and Processes in Crystal Growth Far from Equilibrium (Springer, 2004).
Conte, F., Ninno, D. & Cantele, G. Electronic properties and interlayer coupling of twisted MoS2/NbSe2 heterobilayers. Phys. Rev. B 99, 155429 (2019).
Petrić, M. M. et al. Raman spectrum of Janus transition metal dichalcogenide monolayers WSSe and MoSSe. Phys. Rev. B 103, 035414 (2021).
Petrić, M. M. et al. Nonlinear dispersion relation and out-of-plane second harmonic generation in MoSSe and WSSe Janus monolayers. Adv. Optical Mater. 11, 2300958 (2023).
Yang, B. et al. Effect of distance on photoluminescence quenching and proximity-induced spin–orbit coupling in graphene/WSe2 heterostructures. Nano Lett. 18, 3580–3585 (2018).
Zhou, J. et al. A library of atomically thin metal chalcogenides. Nature 556, 355–359 (2018).
Yi, H. et al. Crossover from Ising- to Rashba-type superconductivity in epitaxial Bi2Se3/monolayer NbSe2 heterostructures. Nat. Mater. 21, 1366–1372 (2022).
Xing, Y. et al. Ising superconductivity and quantum phase transition in macro-size monolayer NbSe2. Nano Lett. 17, 6802–6807 (2017).
Ugeda, M. M. et al. Characterization of collective ground states in single-layer NbSe2. Nat. Phys. 12, 92–97 (2015).
Onishi, S. et al. Selenium capped monolayer NbSe2 for two-dimensional superconductivity studies. Phys. Status Solidi B 253, 2396–2399 (2016).
Nakata, Y. et al. Anisotropic band splitting in monolayer NbSe2: implications for superconductivity and charge density wave. npj 2D Mater. Appl. 2, 12 (2018).
Calavalle, F. et al. Tailoring superconductivity in large-area single-layer NbSe2 via self-assembled molecular adlayers. Nano Lett. 21, 136–143 (2020).
Cho, C.-w. et al. Nodal and nematic superconducting phases in NbSe2 monolayers from competing superconducting channels. Phys. Rev. Lett. 129, 087002 (2022).
Xu, X. et al. Ultrafast epitaxial growth of metre-sized single-crystal graphene on industrial Cu foil. Sci. Bull. 62, 1074–1080 (2017).
Wang, L. et al. Epitaxial growth of a 100-square-centimetre single-crystal hexagonal boron nitride monolayer on copper. Nature 570, 91–95 (2019).
Hu, Z. et al. Rapid and scalable transfer of large-area graphene wafers. Adv. Mater. 35, 2300621 (2023).
Chen, T.-A. et al. Wafer-scale single-crystal hexagonal boron nitride monolayers on Cu (111). Nature 579, 219–223 (2020).
Nan, H. Y. et al. The thermal stability of graphene in air investigated by Raman spectroscopy. J. Raman Spectrosc. 44, 1018–1021 (2013).
Na, Y. S. et al. Modulation of optical and electrical properties in hexagonal boron nitride by defects induced via oxygen plasma treatment. 2D Mater. 8, 045041 (2021).
Grillo, V. & Rotunno, E. STEM_CELL: a software tool for electron microscopy: part I – simulations. Ultramicroscopy 125, 97–111 (2013).
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).
Kresse, G. & Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 59, 1758–1775 (1999).
Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).
Grimme, S. Semiempirical GGA-type density functional constructed with a long-range dispersion correction. J. Comput. Chem. 27, 1787–1799 (2006).
He, W., Geng, D. & Xu, Z. Pattern evolution characterizes the mechanism and efficiency of CVD graphene growth. Carbon 141, 316–322 (2019).
Purdie, D. G. et al. Cleaning interfaces in layered materials heterostructures. Nat. Commun. 9, 5387 (2018).
Acknowledgements
We thank M. Ouyang for helpful discussions. This work was supported by the National Key R&D Program of China (2022YFA1204100), the National Natural Science Foundation of China (62488201) and the Chinese Academy of Sciences (XDB33030100 and XDB30010000). Y.Z. and F.D. acknowledge the startup grant and the High-Talent Grant (SIAT-SE3G0991010, 2023) from the Shenzhen Institute of Advanced Technology. R.G. and W.Z. acknowledge support from the National Natural Science Foundation of China (52373231) and the Beijing Outstanding Young Scientist Program (BJJWZYJH01201914430039). H.H. acknowledges support from the Chinese Academy of Sciences (XDB30000000). W.H. and Z.X. acknowledge support from the National Natural Science Foundation of China (52090032). This work benefited from support and resources from the Electron Microscopy Center at the University of Chinese Academy of Sciences.
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H.-J.G. conceived the idea and designed the project. C.B., Q.Q., K.Z., H.W., K.W. and P.P. synthesized the samples. C.B. performed the Raman, PL and SHG characterizations and conducted the crystal thickness and DGA analyses. R.G., Z.W. and W.Z. performed the STEM/EELS characterizations. Y.Z., H.H. and F.D. performed the DFT calculations. W.H. and Z.X. performed the phase-field simulations. C.B. and H.L. fabricated and measured the devices. C.B., H.L., H.G., F.D. and H.Y. analysed the growth mechanisms. C.B., H.L., W.Z., H.Y. and H.-J.G. wrote the paper with input from all authors.
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The Institute of Physics, Chinese Academy of Sciences filed a Chinese patent application (202111202207.3), which lists C.B., H.Y. and H.-J.G. as the inventors. Other than that, the authors declare no competing interests.
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Bian, C., Zhao, Y., Guzman, R. et al. Atomically precise synthesis and simultaneous heterostructure integration of 2D transition metal dichalcogenides through nano-confinement. Nat. Mater. (2026). https://doi.org/10.1038/s41563-026-02495-9
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DOI: https://doi.org/10.1038/s41563-026-02495-9
