Abstract
Single-crystal alloy thin films (SATFs), featuring highly ordered atomic lattices and superior composition-dependent properties, hold great potential for applications including crystal epitaxy, surface catalysis, and energy conversion. However, their scalable synthesis and practical applications have been hindered by the difficulty of achieving wafer-scale single crystallinity, atomic-scale surface flatness, as well as flexible and uniform control of alloy composition. Here, we developed a surface-energy-compensated technique for synthesizing a series of wafer-scale binary and ternary SATFs with sub-nanometer roughness (minimum roughness lower than 0.2 nm) and uniform, controllable elemental composition with a wide range (5 ~ 50 at%). Furthermore, using CuPtNi(111) ternary SATFs as epitaxial substrates, we achieve wafer-scale synthesis of wrinkle-free graphene single crystals exhibiting fine electronic quality, including a uniform sheet resistance of 552 Ω sq−1 with 4.5% deviation, an ultrahigh carrier mobility up to over half a million cm2 V−1 s−1 at 1.7 K, and well-developed quantum plateaus.
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Relevant data supporting the key findings of this study are available within the article and the Supplementary Information file. All raw data generated during the current study are available from the corresponding authors upon request.
References
Wu, M. et al. Seeded growth of large single-crystal copper foils with high-index facets. Nature 581, 406–410 (2020).
Jin, S. et al. Colossal grain growth yields single-crystal metal foils by contact-free annealing. Science 362, 1021–1025 (2018).
Karaman, C. O., Bykov, A. Y., Kiani, F., Tagliabue, G. & Zayats, A. V. Ultrafast hot-carrier dynamics in ultrathin monocrystalline gold. Nat. Commun. 15, 703 (2024).
Chen, H. et al. Oxidization-temperature-triggered rapid preparation of large-area single-crystal Cu(111) foil. Adv. Mater. 35, 2209755 (2023).
Cui, Z., Wong, A. J.-W., Janik, M. J. & Co, A. C. Cation effects on CO2 reduction catalyzed by single-crystal and polycrystalline gold under well-defined mass transport conditions. Sci. Adv. 11, eadr6465 (2025).
Pérez-Gallent, E., Marcandalli, G., Figueiredo, M. C., Calle-Vallejo, F. & Koper, M. T. M. Structure- and potential-dependent cation effects on CO reduction at copper single-crystal electrodes. J. Am. Chem. Soc. 139, 16412–16419 (2017).
Yuan, G. et al. Proton-assisted growth of ultra-flat graphene films. Nature 577, 204–208 (2020).
Nguyen, V. L. et al. Layer-controlled single-crystalline graphene film with stacking order via Cu-Si alloy formation. Nat. Nanotechnol. 15, 861–867 (2020).
Jiang, J., Ding, W., Li, W. & Wei, Z. Freestanding single-atom-layer Pd-based catalysts: oriented splitting of energy bands for unique stability and activity. Chem 6, 431–447 (2020).
Yao, J. & Yang, G. 2D layered material alloys: synthesis and application in electronic and optoelectronic devices. Adv. Sci. 9, 2103036 (2022).
Wu, T. et al. Fast growth of inch-sized single-crystalline graphene from a controlled single nucleus on Cu-Ni alloys. Nat. Mater. 15, 43–47 (2016).
Wang, Y. et al. Ultraflat single-crystal hexagonal boron nitride for wafer-scale integration of a 2D-compatible high-κ metal gate. Nat. Mater. 23, 1495–1501 (2024).
Wang, M. et al. Single-crystal, large-area, fold-free monolayer graphene. Nature 596, 519–524 (2021).
Zhang, X. et al. Epitaxial growth of 6 in. single-crystalline graphene on a Cu/Ni (111) film at 750 °C via chemical vapor deposition. Small 15, 1805395 (2019).
Huang, M. et al. Large-area single-crystal AB-bilayer and ABA-trilayer graphene grown on a Cu/Ni(111) foil. Nat. Nanotechnol. 15, 289–295 (2020).
Sun, L. et al. Toward epitaxial growth of misorientation-free graphene on Cu(111) foils. ACS Nano 16, 285–294 (2022).
Yao, W. et al. Bottom-up-etching-mediated synthesis of large-scale pure monolayer graphene on cyclic-polishing-annealed Cu(111). Adv. Mater. 34, 2108608 (2022).
Deng, B. et al. Wrinkle-free single-crystal graphene wafer grown on strain-engineered substrates. ACS Nano 11, 12337–12345 (2017).
Kim, S. J. et al. Flat-surface-assisted and self-regulated oxidation resistance of Cu(111). Nature 603, 434–438 (2022).
Camacho, J. M. & Oliva, A. I. Surface and grain boundary contributions in the electrical resistivity of metallic nanofilms. Thin Solid Films 515, 1881–1885 (2006).
Kim, K. et al. Extremely flat metal films implemented by surface roughness transfer for flexible electronics. RSC Adv. 8, 10883–10888 (2018).
Tian, B. et al. Ultraflat Cu(111) foils by surface acoustic wave-assisted annealing. Nat. Commun. 15, 9488 (2024).
Zheng, L. et al. Uniform thin ice on ultraflat graphene for high-resolution cryo-EM. Nat. Methods 20, 123–130 (2023).
Luo, D. et al. Folding and fracture of single-crystal graphene grown on a Cu(111) foil. Adv. Mater. 34, 2110509 (2022).
Zhao, Y. et al. Large-area transfer of two-dimensional materials free of cracks, contamination and wrinkles via controllable conformal contact. Nat. Commun. 13, 4409 (2022).
Ha, T. et al. Coherent consolidation of trillions of nucleations for mono-atom step-level flat surfaces. Nat. Commun. 14, 685 (2023).
Kim, S. J. et al. Color of copper/copper oxide. Adv. Mater. 33, 2007345 (2021).
Tang, J. et al. Ultrafast growth of wafer-scale fold-free bilayer graphene. Nano Res. 16, 10684–10689 (2023).
Miller, D. L., Keller, M. W., Shaw, J. M., Chiaramonti, A. N. & Keller, R. R. Epitaxial (111) films of Cu, Ni, and CuxNiy on α-Al2O3(0001) for graphene growth by chemical vapor deposition. J. Appl. Phys. 112 (2012).
Burton, O. J. et al. Integrated wafer scale growth of single crystal metal films and high-quality graphene. ACS Nano 14, 13593–13601 (2020).
Oh, S., Scheu, C., Wagner, T., Tchernychova, E. & Ruhle, M. Epitaxy and bonding of Cu films on oxygen-terminated α-Al2O3(0001). Surf. Acta Mater. 54, 2685–2696 (2006).
Han, G. H. et al. Influence of copper morphology in forming nucleation seeds for graphene growth. Nano Lett. 11, 4144–4148 (2011).
Luo, Z. et al. Effect of substrate roughness and feedstock concentration on growth of wafer-scale graphene at atmospheric pressure. Chem. Mater. 23, 1441–1447 (2011).
Zhu, Y. et al. Controlled growth of single-crystal graphene wafers on twin-boundary-free Cu(111) substrates. Adv. Mater. 36, 2308802 (2024).
Chen, T.-A. et al. Wafer-scale single-crystal hexagonal boron nitride monolayers on Cu(111). Nature 579, 219–223 (2020).
Deng, B. et al. Scalable and ultrafast epitaxial growth of single-crystal graphene wafers for electrically tunable liquid-crystal microlens arrays. Sci. Bull. 64, 659–668 (2019).
Amram, D., Klinger, L. & Rabkin, E. Anisotropic hole growth during solid-state dewetting of single-crystal Au-Fe thin films. Acta Mater. 60, 3047–3056 (2012).
Dierner, M. et al. Influence of Au alloying on solid state dewetting kinetics and texture evolution of Ag and Ni thin films. Surf. Interf. 46, 1–8 (2024).
Herz, A. et al. Solid-state dewetting of Au-Ni bi-layer films mediated through individual layer thickness and stacking sequence. Appl. Surf. Sci. 444, 505–510 (2018).
Wen, Y.-N. & Zhang, J.-M. Surface energy calculation of the fcc metals by using the MAEAM. Solid State Commun. 144, 163–167 (2007).
Liu, H., Valanoor, N., Bogle, K. & Cheng, X. An empirical method for surface energy anisotropy determination in high symmetry crystals. ACS Omega 10, 45278–45289 (2025).
Singh-Miller, N. & Marzari, N. Surface energies, work functions, and surface relaxations of low-index metallic surfaces from first principles. Phys. Rev. B. 80, 235407 (2009).
Gioria, E. et al. CuNi nanoalloys with tunable composition and oxygen defects for the enhancement of the oxygen evolution reaction. Angew. Chem. Int. Ed. 62, e202217888 (2023).
Luo, D. et al. Adlayer-free large-area single crystal graphene grown on a Cu(111) foil. Adv. Mater. 31, 1903615 (2019).
Miller, D. L. et al. Giant secondary grain growth in Cu films on sapphire. AIP Adv. 3, 082105 (2013).
Lee, I.-J. et al. Epitaxial growth and characterization of Cu thin films deposited on Al2O3(0001) substrates by magnetron sputtering. Mater. Lett. 299, 130119 (2021).
Hÿtch, M. J., Putaux, J.-L. & Pénisson, J.-M. Measurement of the displacement field of dislocations to 0.03 Å by electron microscopy. Nature 423, 270–273 (2003).
Wang, X., Yuan, Q., Li, J. & Ding, F. The transition metal surface dependent methane decomposition in graphene chemical vapor deposition growth. Nanoscale 9, 11584–11589 (2017).
Zhao, C. & Ding, F. Temperature-dependent graphene wrinkle formation: A theoretical study. Sci. China Mater. 67, 2210–2216 (2024).
Yi, D. et al. What drives metal-surface step bunching in graphene chemical vapor deposition? Phys. Rev. Lett. 120, 246101–246105 (2018).
Yu, H. et al. Eight in. wafer-scale epitaxial monolayer MoS2. Adv. Mater. 36, 2402855 (2024).
Taniguchi, T. et al. Revisiting the two-dimensional structure and reduction process of graphene oxide with in-plane X-ray diffraction. Carbon 202, 26–35 (2023).
Li, X. et al. Single-crystal two-dimensional material epitaxy on tailored non-single-crystal substrates. Nat. Commun. 13, 1773 (2022).
Amontree, J. et al. Reproducible graphene synthesis by oxygen-free chemical vapour deposition. Nature 630, 636–642 (2024).
Ferrari, A. C. & Basko, D. M. Raman spectroscopy as a versatile tool for studying the properties of graphene. Nat. Nanotechnol. 8, 235–246 (2013).
Giambra, M. A. et al. Wafer-scale integration of graphene-based photonic devices. ACS Nano 15, 3171–3187 (2021).
Canto, B. et al. Multi-project wafer runs for electronic graphene devices in the European 2D-Experimental Pilot Line project. Nat. Commun. 16, 1417 (2025).
Lee, S. et al. Contact resistivity in edge-contacted graphene field effect transistors. Adv. Electron. Mater. 8, 2101169 (2022).
Banszerus, L. et al. Ultrahigh-mobility graphene devices from chemical vapor deposition on reusable copper. Sci. Adv. 1, e1500222 (2015).
Moon, J.-Y. et al. Layer-engineered large-area exfoliation of graphene. Sci. Adv. 6, eabc6601 (2020).
Dean, C. R. et al. Boron nitride substrates for high-quality graphene electronics. Nat. Nanotechnol. 5, 722–726 (2010).
Wang, L. et al. One-dimensional electrical contact to a two-dimensional material. Science 342, 614–617 (2013).
Ki, D.-K. & Morpurgo, A. F. High-quality multiterminal suspended graphene devices. Nano Lett. 13, 5165–5170 (2013).
Novoselov, K. S. et al. Room-temperature quantum Hall effect in graphene. Science 315, 1379–1379 (2007).
Feldman, B. E., Martin, J. & Yacoby, A. Broken-symmetry states and divergent resistance in suspended bilayer graphene. Nat. Phys. 5, 889–893 (2009).
Gao, X. et al. Integrated wafer-scale ultra-flat graphene by gradient surface energy modulation. Nat. Commun. 13, 5410 (2022).
Zhang, J. et al. Clean transfer of large graphene single crystals for high-intactness suspended membranes and liquid cells. Adv. Mater. 29, 1700639 (2017).
Pavesi, M., Parisini, A., Calvi, P., Bosio, A. & Fornari, R. Effects of the interface properties on the performance of UV-C photoresistors: gallium oxide as case study. Sensors 25, 345 (2025).
Sun, X. et al. Correlated states in doubly-aligned hBN/graphene/hBN heterostructures. Nat. Commun. 12, 7196 (2021).
Acknowledgements
This work was supported by the National Natural Science Foundation of China (Nos. T2188101, 52202033, and 52372038), the National Key Research and Development Program of China (No. 2022YFA1204900), Beijing Natural Science Foundation (No. 2252064), the Beijing National Laboratory for Molecular Sciences (No. BNLMS-CXTD−202001), and Jiangsu Materials Science Association (No. JSTJ−2024-047). We acknowledge the Electron Microscopy Laboratory of Peking University, China, for the use of JEM-ARM200F NEOARM transmission electron microscopy. We thank the Center for Physicochemical Analysis and Measurement, Institute of Chemistry, Chinese Academy of Sciences, for assistance with XRD characterization. We thank the engineer Chong Guo, Analysis Center, Department of Chemistry, Tsinghua University, for her help with the TOF-SIMS test.
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J.S., S.L., Z.S., and Y.S. contributed equally to this work. Z.L. and K.J. conceived the experiment. Z.L. and K.J. supervised the project. J.S., S.L., Y.S., and G.G. conducted the fabrication of SATFs and CVD growth of graphene. J.S., S.L., Y.S., G.G., S.W., Y.G., D.Z., W.C., and B.Y. took and analyzed the OM, EBSD, AFM, XRD, and SAED data. M.Y.L. and M.X.L. conducted the STM characterization. X.M. conducted the STEM and EDS characterization. W.C. and J.Z. conducted the Raman measurements. S.W. conducted the in-plane XRD characterization. J.S. and Y.S. conducted the transfer of graphene. Z.S., J.L., and L.L. performed device fabrication and electrical measurements. J.S., G.G., and B.J. conducted sheet resistance measurements. A.C. designed the automatic OM system. H.L. and X.S. conducted the DFT calculations. The manuscript was written by Z.L. and K.J. All authors discussed the results and wrote the manuscript.
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Shao, J., Li, S., Shi, Z. et al. Surface-energy-compensated fabrication of single-crystal alloy films with atomic-scale flatness. Nat Commun (2026). https://doi.org/10.1038/s41467-025-68196-0
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DOI: https://doi.org/10.1038/s41467-025-68196-0


