Signatures of polarized chiral spin disproportionation in rare earth nickelates

Jiarui Li; Robert J. Green; Claribel Domínguez; Abraham Levitan; Yi Tseng; Sara Catalano; Jennifer Fowlie; Ronny Sutarto; Fanny Rodolakis; Lucas Korol; Jessica L. McChesney; John W. Freeland; Dirk Van der Marel; Marta Gibert; Riccardo Comin

doi:10.1038/s41467-024-51576-3

Signatures of polarized chiral spin disproportionation in rare earth nickelates

Jiarui Li^*, Robert J. Green, Claribel Domínguez, Abraham Levitan, Yi Tseng, Sara Catalano, Jennifer Fowlie, Ronny Sutarto, Fanny Rodolakis, Lucas Korol, Jessica L. McChesney, John W. Freeland, Dirk Van der Marel, Marta Gibert, Riccardo Comin^*

^*Corresponding author for this work

Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

Abstract

In rare earth nickelates (RENiO₃), electron-lattice coupling drives a concurrent metal-to-insulator and bond disproportionation phase transition whose microscopic origin has long been the subject of active debate. Of several proposed mechanisms, here we test the hypothesis that pairs of self-doped ligand holes spatially condense to provide local spin moments that are antiferromagnetically coupled to Ni spins. These singlet-like states provide a basis for long-range bond and spiral spin order. Using magnetic resonant X-ray scattering on NdNiO₃ thin films, we observe the chiral nature of the spin-disproportionated state, with spin spirals propagating along the crystallographic (101)_ortho direction. These spin spirals are found to preferentially couple to X-ray helicity, establishing the presence of a hitherto-unobserved macroscopic chirality. The presence of this chiral magnetic configuration suggests a potential multiferroic coupling between the noncollinear magnetic arrangement and improper ferroelectric behavior as observed in prior studies on NdNiO₃ (101)_ortho films and RENiO₃ single crystals. Experimentally-constrained theoretical double-cluster calculations confirm the presence of an energetically stable spin-disproportionated state with Zhang-Rice singlet-like combinations of Ni and ligand moments.

Original language	English (US)
Article number	7427
Journal	Nature communications
Volume	15
Issue number	1
DOIs	https://doi.org/10.1038/s41467-024-51576-3
State	Published - Dec 2024

Funding

We thank G.A. Sawatzky and J.M. Triscone for fruitful discussion. This material is based upon work supported by the Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DE-SC0019126 (X-ray scattering measurements and form factor analysis). RJG was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC). M.G. acknowledges the Swiss National Science Foundation (SNSF) under Project No. PP00P2_170564. Part of the research described in this paper was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), NSERC, the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science user facility at Argonne National Laboratory and is based on research supported by the U.S. DOE Office of Science-Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The work of DvdM was supported by the Swiss National Science Foundation through project 200020-179157.\u00A0The authors acknowledge the MIT SuperCloud and Lincoln Laboratory Supercomputing Center for providing computing resources that have contributed to the research results reported within this paper. We thank G.A. Sawatzky and J.M. Triscone for fruitful discussion. This material is based upon work supported by the Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DE-SC0019126 (X-ray scattering measurements and form factor analysis). RJG was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC). M.G. acknowledges the Swiss National Science Foundation (SNSF) under Project No. PP00P2_170564. Part of the research described in this paper was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), NSERC, the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science user facility at Argonne National Laboratory and is based on research supported by the U.S. DOE Office of Science-Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The work of DvdM was supported by the Swiss National Science Foundation through project 200020-179157. The authors acknowledge the MIT SuperCloud and Lincoln Laboratory Supercomputing Center for providing computing resources that have contributed to the research results reported within this paper.

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

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10.1038/s41467-024-51576-3

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Li, J., Green, R. J., Domínguez, C., Levitan, A., Tseng, Y., Catalano, S., Fowlie, J., Sutarto, R., Rodolakis, F., Korol, L., McChesney, J. L., Freeland, J. W., Van der Marel, D., Gibert, M., & Comin, R. (2024). Signatures of polarized chiral spin disproportionation in rare earth nickelates. Nature communications, 15(1), Article 7427. https://doi.org/10.1038/s41467-024-51576-3

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abstract = "In rare earth nickelates (RENiO3), electron-lattice coupling drives a concurrent metal-to-insulator and bond disproportionation phase transition whose microscopic origin has long been the subject of active debate. Of several proposed mechanisms, here we test the hypothesis that pairs of self-doped ligand holes spatially condense to provide local spin moments that are antiferromagnetically coupled to Ni spins. These singlet-like states provide a basis for long-range bond and spiral spin order. Using magnetic resonant X-ray scattering on NdNiO3 thin films, we observe the chiral nature of the spin-disproportionated state, with spin spirals propagating along the crystallographic (101)ortho direction. These spin spirals are found to preferentially couple to X-ray helicity, establishing the presence of a hitherto-unobserved macroscopic chirality. The presence of this chiral magnetic configuration suggests a potential multiferroic coupling between the noncollinear magnetic arrangement and improper ferroelectric behavior as observed in prior studies on NdNiO3 (101)ortho films and RENiO3 single crystals. Experimentally-constrained theoretical double-cluster calculations confirm the presence of an energetically stable spin-disproportionated state with Zhang-Rice singlet-like combinations of Ni and ligand moments.",

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AU - Fowlie, Jennifer

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Signatures of polarized chiral spin disproportionation in rare earth nickelates

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