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 Marel, Marta Gibert and Riccardo Comin ()
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Jiarui Li: Massachusetts Institute of Technology
Robert J. Green: University of Saskatchewan
Claribel Domínguez: University of Geneva
Abraham Levitan: Massachusetts Institute of Technology
Yi Tseng: Massachusetts Institute of Technology
Sara Catalano: University of Geneva
Jennifer Fowlie: University of Geneva
Ronny Sutarto: Canadian Light Source
Fanny Rodolakis: Argonne National Laboratory
Lucas Korol: University of Saskatchewan
Jessica L. McChesney: Argonne National Laboratory
John W. Freeland: Argonne National Laboratory
Dirk Marel: University of Geneva
Marta Gibert: Vienna University of Technology
Riccardo Comin: Massachusetts Institute of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-6

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-51576-3

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