Local site behavior of the 5$d$ and 4$f$ ions in the frustrated pyrochlore Ho2Os2O7

Calder, Stuart; Zhao, Zhiying; Upton, Mary H.; Yan, Jianqiang

doi:10.1103/physrevb.109.054408

Title: Local site behavior of the 5$$d$$ and 4$$f$$ ions in the frustrated pyrochlore Ho₂Os₂O₇

Journal Article · Thu Feb 08 00:00:00 EST 2024 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.109.054408· OSTI ID:2317758

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

The pyrochlore osmate Ho₂Os₂O₇ is a candidate material for a fragile J=0 local singlet ground state, however little is known regarding the single-ion behavior of either the Os or Ho ions. To address this we present polarized neutron powder diffraction (PNPD) and resonant inelastic x-ray scattering (RIXS) measurements that separately probe the local site behavior of the Os and Ho ions. The PNPD results are dominated by Ho³⁺ scattering and the analysis reveals local site susceptibility behavior consistent with spin ice materials. Complimentary unpolarized neutron powder diffraction show an ordered spin ice ground state in an applied magnetic field. To isolate the Os⁴⁺ single-ion behavior we present resonant inelastic x-ray scattering (RIXS) measurements at the osmium L-edge. Analysis of the RIXS spectra parameterize the spin-orbit coupling (0.35 eV), Hund’s coupling (0.27 eV) and trigonal distortion (-0.17 eV). Here, the results are considered within the context of a J=0 model and possible departures from this through structural distortions, excitonic interactions and 5d-4f interactions between the Os ion and the surrounding Ho lattice. The experimental methodology employed highlights the complimentary information available in rare earth based 5d pyrochlores from distinct neutron and x-ray scattering techniques that allow for the isolation and determination of the behavior of the different ions.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

OSTI ID:: 2317758

Journal Information:: Physical Review. B, Vol. 109, Issue 5; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Local site behavior of the 5$$d$$ and 4$$f$$ ions in the frustrated pyrochlore Ho2Os2O7

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Title: Local site behavior of the 5$$d$$ and 4$$f$$ ions in the frustrated pyrochlore Ho₂Os₂O₇