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Antiferromagnetic metal phase in an electron-doped rare-earth nickelate

Nature Physics volume 19, pages 522–528 (2023)Cite this article

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Abstract

Long viewed as passive elements, antiferromagnetic materials have emerged as promising candidates for spintronic devices due to their insensitivity to external fields and potential for high-speed switching. Recent work exploiting spin and orbital effects has identified ways to electrically control and probe the spins in metallic antiferromagnets, especially in non-collinear or non-centrosymmetric spin structures. The rare-earth nickelate NdNiO3 is known to be a non-collinear antiferromagnet in which the onset of antiferromagnetic ordering is concomitant with a transition to an insulating state. Here we find that for low electron doping, the magnetic order on the nickel site is preserved, whereas electronically, a new metallic phase is induced. We show that this metallic phase has a Fermi surface that is mostly gapped by an electronic reconstruction driven by bond disproportionation. Furthermore, we demonstrate the ability to write to and read from the spin structure via a large zero-field planar Hall effect. Our results expand the already rich phase diagram of rare-earth nickelates and may enable spintronics applications in this family of correlated oxides.

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Fig. 1: Structural and electrical characterization of CexNd1−xNiO3 thin films.
Fig. 2: Electronic transition in CexNd1−xNiO3 viewed by ARPES.
Fig. 3: RXS data and phase diagram of CexNd1−xNiO3.
Fig. 4: Large ZF-PHE in a metallic antiferromagnetic nickelate.

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The data presented in the figures and other findings of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.

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Acknowledgements

This work is supported by the STC Center for Integrated Quantum Materials, NSF grant no. DMR-1231319. Materials growth and simulations were supported by the National Science Foundation (Platform for the Accelerated Realization, Analysis, and Discovery of Interface Materials (PARADIM)) under cooperative agreement no. DMR-2039380. This work used resources of the Advanced Light Source, which is a US Department of Energy (DOE) Office of Science User Facility under contract no. DE-AC02-05CH11231. The ARPES work was partially funded by the US DOE, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under contract no. DE-AC02-05CH11231 (Ultrafast Materials Program KC2203). Electron microscopy was carried out through the use of MIT.nano facilities at the Massachusetts Institute of Technology. Additional electron microscopy work was performed at Harvard University’s Center for Nanoscale Systems, a member of the National Nanotechnology Coordinated Infrastructure Network, supported by the NSF under grant no. 2025158. A portion of this research used resources at the Spallation Neutron Source (SNS), a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory (ORNL). ORNL is managed by UT-Battelle LLC for DOE’s Office of Science, the single largest supporter of basic research in the physical sciences in the US. This manuscript has been authored by UT-Battelle LLC, under contract DE-AC05-00OR22725 with the US DOE. The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). Device fabrication work was performed at Harvard University’s Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network (NNCI), supported by the National Science Foundation under NSF grant no. 1541959. Any mention of commercial products within this paper is for information only; it does not imply recommendation or endorsement by NIST. Work at the NCNR was supported by the Department of Commerce. W.D.R. acknowledges support from the Department of Commerce. S.D. acknowledges support from the NSF Graduate Research Fellowship grant no. DGE-1745303. G.A.P. acknowledges support from the Paul & Daisy Soros Fellowship for New Americans and from the NSF Graduate Research Fellowship grant no. DGE-1745303. H.E.-S. and I.E.B. were supported by The Rowland Institute at Harvard. J.N. acknowledges support from the Swiss National Science Foundation under project no. P2EZP2_195686. C.T. acknowledges support from the Swiss National Science Foundation under project no. P2EZP2_191801. S.-Y.X. and C.T. were supported by NSF Career (Harvard fund 129522) DMR-2143177. H.L. and A.S.B. acknowledge support from NSF grant no. DMR-2045826 and the ASU Research Computing Center for the high-performance computing resources. J.A.M. acknowledges support from the Packard Foundation and Gordon and Betty Moore Foundation’s EPiQS Initiative (grant GBMF6760).

Author information

Author notes

  1. These authors contributed equally: Qi Song, Spencer Doyle.

Authors and Affiliations

  1. Department of Physics, Harvard University, Cambridge, MA, USA

    Qi Song, Spencer Doyle, Grace A. Pan, Dan Ferenc Segedin, Denisse Córdova Carrizales, Johanna Nordlander, James R. Ehrets, Zubia Hasan, Charles M. Brooks & Julia A. Mundy

  2. The Rowland Institute at Harvard, Harvard University, Cambridge, MA, USA

    Ismail El Baggari & Hesham El-Sherif

  3. Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USA

    Christian Tzschaschel & Su-Yang Xu

  4. Department of Physics, Arizona State University, Tempe, AZ, USA

    Jyoti Krishna, Chase Hanson, Harrison LaBollita & Antia S. Botana

  5. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Aaron Bostwick, Chris Jozwiak, Eli Rotenberg, Alpha T. N’Diaye & Padraic Shafer

  6. Department of Physics, University of California at Berkeley, Berkeley, CA, USA

    Alessandra Lanzara & Luca Moreschini

  7. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Alessandra Lanzara & Luca Moreschini

  8. NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD, USA

    Colin A. Heikes & William D. Ratcliff

  9. Joint Quantum Institute, National Institute of Standards and Technology and the University of Maryland, Gaithersburg, MD, USA

    Colin A. Heikes

  10. Neutron Scattering Division, Oak Ridge National Lab, Oak Ridge, TN, USA

    Yaohua Liu

  11. Second Target Station, Oak Ridge National Laboratory, Oak Ridge, TN, USA

    Yaohua Liu

  12. Platform for the Accelerated Realization, Analysis and Discovery of Interface Materials (PARADIM), Cornell University, Ithaca, NY, USA

    Hanjong Paik, Betül Pamuk & Luca Moreschini

  13. School of Electrical and Computer Engineering, University of Oklahoma, Norman, OK, USA

    Hanjong Paik

  14. Center for Quantum Research and Technology (CQRT), University of Oklahoma, Norman, OK, USA

    Hanjong Paik

  15. Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI, USA

    John T. Heron

  16. Department of Materials Science and Engineering, University of Maryland, College Park, MD, USA

    William D. Ratcliff

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  1. Qi Song
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Contributions

Q.S., G.A.P., C.M.B. and J.A.M. synthesized the thin films with assistance from H.P. Q.S. and L.M. performed the ARPES measurements with support from A.S.B., C.J., E.R., D.F.S., Z.H. and A.L. S.D., Q.S. and J.A.M. performed the electrical measurements with assistance from J.T.H. H.E.-S. and I.E. characterized the samples with scanning transmission electron microscopy. G.A.P., S.D., J.R.E., D.F.S., Q.S., D.C.C., A.T.N. and P.S. performed the X-ray spectroscopy and scattering measurements. C.A.H., Y.L. and W.D.R. performed the neutron diffraction measurements. J.N., C.T. and S.-Y.X. performed the second-harmonic generation measurements. B.P. and A.S.B. performed the DFT calculations. J.A.M. conceived and guided the study. Q.S., S.D., L.M. and J.A.M. wrote the manuscript with discussion and contributions from all authors.

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Correspondence to Luca Moreschini or Julia A. Mundy.

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Supplementary Figs. 1–22 and discussion.

Source data

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Transport source data.

Source Data Fig. 2

Angle-resolved photoemission spectroscopy source data.

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Resonant x-ray scattering source data.

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Planar Hall effect source data.

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Song, Q., Doyle, S., Pan, G.A. et al. Antiferromagnetic metal phase in an electron-doped rare-earth nickelate. Nat. Phys. 19, 522–528 (2023). https://doi.org/10.1038/s41567-022-01907-2

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