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Synthesis of superconducting freestanding infinite-layer nickelate heterostructures on the millimetre scale

Nature Synthesis volume 4, pages 573–581 (2025)Cite this article

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Abstract

The development of superconductivity in infinite-layer nickelates through hole-doping relies on the controlled synthesis of Ni in a high oxidation state, followed by topotactic reduction to a very low oxidation state. So far, superconductivity has been realized only in epitaxial thin films. Here we integrate these techniques with heterostructures that include an epitaxial soluble buffer layer, enabling the release of freestanding (Nd,Sr)NiO2 heterostructures. The released heterostructures exhibit comparable structural and electronic properties to those of optimized thin films, with lateral dimensions ranging from millimetres to ~100 μm, depending on the degree of strain released with respect to the initial substrate. The changes in the superconducting transition temperature upon release of the heterostructure mirror those reported for variations in substrate and pressure, suggesting a common underlying response to strain in the infinite-layer nickelate superconductivity. These freestanding structures will facilitate a range of experimental studies without the constraints of substrates.

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Fig. 1: Schematic diagrams illustrating the synthesis of freestanding infinite-layer nickelate heterostructures and representative images of the sample at various steps.
Fig. 2: Structural characterization of nickelate heterostructures on substrates and in freestanding form.
Fig. 3: STEM images of an STO/Nd0.8Sr0.2NiO2/STO heterostructure transferred onto a SiNx TEM window.
Fig. 4: Electrical and magnetic characteristics of the infinite-layer nickelate heterostructures on substrates and in their freestanding form.
Fig. 5: Comparison of the present results with previous reports on (Pr or Nd)1−xSrxNiO2 thin films.

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All source data supporting the findings of this study are provided. Source data are provided with this paper.

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Acknowledgements

We acknowledge D. Li and V. Harbola for their contributions to the initial stage of this work, W. J. Kim, E. K. Ko and A. Vailionis for assistance with RSM measurements, and E. K. Ko, J. Fowlie, K. J. Crust and J. Wang for critical reading of the manuscript. This work was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering (contract no. DE-AC02-76SF00515) and the Gordon and Betty Moore Foundation’s Emergent Phenomena in Quantum Systems Initiative (grant no. GBMF9072, synthesis equipment). Electron microscopy by L.B., B.H.G., D.A.M. and L.F.K. was supported by Platform for the Accelerated Realization, Analysis and Discovery of Interface Materials (PARADIM) through NSF DMR-2039380 with additional support by the Department of Defense Air Force Office of Scientific Research (grant no. FA 9550-16-1-0305) and the Packard Foundation. This work made use of a Helios focused ion beam set-up supported by the NSF (grant no. DMR-1539918) and the Cornell Center for Materials Research Shared Facilities, which are supported through the NSF MRSEC programme (grant no. DMR-1719875). The Thermo Fisher Spectra 300 X-CFEG system was acquired with support from PARADIM, an NSF MIP (no. DMR-2039380) and Cornell University. The FEI Titan Themis was acquired through NSF-MRI-1429155, with additional support from Cornell University, the Weill Institute and the Kavli Institute at Cornell. This work is dedicated to L.F.K., who passed away on 24 June 2023.

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Author notes

  1. Kyuho Lee

    Present address: Department of Physics, Massachusetts Institute of Technology, Cambridge, MA, USA

  2. Berit H. Goodge

    Present address: Max Planck Institute for Chemical Physics of Solids, Dresden, Germany

  3. These authors contributed equally: Yonghun Lee, Xin Wei.

Authors and Affiliations

  1. Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Yonghun Lee, Xin Wei, Yijun Yu, Kyuho Lee, Shannon P. Harvey, Bai Yang Wang, Wei-Sheng Lee, Srinivas Raghu & Harold Y. Hwang

  2. Department of Applied Physics, Stanford University, Stanford, CA, USA

    Yonghun Lee, Yijun Yu, Shannon P. Harvey & Harold Y. Hwang

  3. Department of Physics, Stanford University, Stanford, CA, USA

    Xin Wei, Kyuho Lee, Bai Yang Wang & Srinivas Raghu

  4. School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA

    Lopa Bhatt, Berit H. Goodge, David A. Muller & Lena F. Kourkoutis

  5. Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY, USA

    Berit H. Goodge, David A. Muller & Lena F. Kourkoutis

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Contributions

Y.L., X.W. and K.L. synthesized the nickelate freestanding heterostructures. Y.L., X.W. and Y.Y. performed transport measurements. Y.L. and X.W. conducted XRD characterizations. L.B., B.H.G., D.A.M. and L.F.K. conducted STEM measurements. S.P.H. and B.Y.W. performed the mutual-inductance measurements. Y.L., X.W., Y.Y. and H.Y.H. wrote the manuscript with input from all authors. D.A.M., L.F.K., W.-S.L., S.R. and H.Y.H. supervised the project.

Corresponding authors

Correspondence to Yonghun Lee, Xin Wei or Harold Y. Hwang.

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Nature Synthesis thanks the anonymous reviewers for their contribution to the peer review of this work. Primary Handling Editor: Alison Stoddart, in collaboration with the Nature Synthesis team.

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Supplementary information

Source data

Source Data Fig. 2 (download XLSX )

XRD θ-2θ symmetric scan data, Reciprocal space mapping data.

Source Data Fig. 3 (download XLSX )

Cross-sectional ADF image intensity profiles.

Source Data Fig. 4 (download XLSX )

Temperature-dependent resistivity of as-grown and freestanding heterostructure. Temperature-dependent real and imaginary components of a.c. voltage from the mutual-inductance measurement.

Source Data Fig. 5 (download XLSX )

Table of Tc, onset versus a-axis lattice constants.

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Lee, Y., Wei, X., Yu, Y. et al. Synthesis of superconducting freestanding infinite-layer nickelate heterostructures on the millimetre scale. Nat. Synth 4, 573–581 (2025). https://doi.org/10.1038/s44160-024-00714-2

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