Electronic structure of the frustrated diamond lattice magnet NiRh2O4

Zager, B.; Chamorro, J. R.; Ge, L.; Bahrami, F.; Bisogni, V.; Pelliciari, J.; Li, J.; Fabbris, G.; McQueen, T. M.; Mourigal, M.; Plumb, K. W.

doi:10.1103/physrevb.106.045134

Title: Electronic structure of the frustrated diamond lattice magnet NiRh 2 O 4

Journal Article · Mon Jul 25 00:00:00 EDT 2022 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.106.045134· OSTI ID:1889167

^[1]; Chamorro, J. R. ^[2]; Ge, L. ^[3]; Bahrami, F. ^[4];

^[5]; Pelliciari, J. ^[5]; Li, J. ^[5];

^[6]; McQueen, T. M. ^[2];

^[3];

^[1]

Brown University, Providence, RI (United States)
Johns Hopkins University, Baltimore, MD (United States)
Georgia Institute of Technology, Atlanta, GA (United States)
Boston College, Chestnut Hill, MA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Argonne National Laboratory (ANL), Lemont, IL (United States)

We report the A -site spinel NiRh₂O₄ is the only known realization of a spin-1 diamond lattice magnet and is predicted to host unconventional magnetic phenomena driven by frustrated nearest and next-nearest neighbor exchange as well as orbital degeneracy. Previous works found no sign of magnetic order but found a gapped dispersive magnetic excitation indicating a possible valence bond magnetic ground state. However, the presence of many competing low energy degrees of freedom and limited empirical microscopic constraints complicates further analysis. Here we carry out resonant inelastic x-ray scattering (RIXS), x-ray absorption spectroscopy (XAS), and inelastic neutron scattering (INS) to characterize the local electronic structure and lattice dynamics of NiRh₂O₄. The RIXS data can be partly described by a single-ion model for tetrahedrally coordinated Ni²⁺ and indicates a tetragonal distortion Δt₂ = 70 meV that splits the t₂ orbitals into a high energy orbital singlet and lower energy orbital doublet. We identify features of the RIXS spectra that are consistent with a Rh-Ni two-site excitation indicating strong metal-metal hybridization mediated by oxygen in NiRh₂O₄. We also identify signatures of electron-phonon coupling through the appearance of phonon sidebands that dress crystal field excitations. These results establish the key energy scales relevant to the magnetism in NiRh₂O₄ and further demonstrate that covalency and lattice dynamics play essential roles in controlling the magnetic ground states of A -site spinels.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; SC002165; SC0019331; DMR-175018; AC02-06CH11357

OSTI ID:: 1889167

Alternate ID(s):: OSTI ID: 1908130

Report Number(s):: BNL-223418-2022-JAAM; TRN: US2310052

Journal Information:: Physical Review. B, Vol. 106, Issue 4; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Electronic structure of the frustrated diamond lattice magnet NiRh 2 O 4

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