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Signatures of polarized chiral spin disproportionation in rare earth nickelates

Journal Article · · Nature Communications
 [1];  [2];  [3];  [4];  [4];  [3];  [3];  [5];  [6];  [7];  [6];  [6];  [3];  [8];  [4]
  1. Massachusetts Institute of Technology, Cambridge, MA (United States); Massachusetts Institute of Technology
  2. University of Saskatchewan (Canada); University of British Columbia (Canada)
  3. University of Geneva (Switzerland)
  4. Massachusetts Institute of Technology, Cambridge, MA (United States)
  5. Canadian Light Source, Saskatoon, SK (Canada)
  6. Argonne National Laboratory (ANL), Argonne, IL (United States)
  7. University of Saskatchewan (Canada)
  8. Vienna University of Technology (Austria)
+ Show Author Affiliations
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
Research Organization:
Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357; SC0019126
OSTI ID:
2439256
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

75 CONDENSED MATTER PHYSICS
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