English

Electronic structure of the frustrated diamond lattice magnet NiRh$_2$O$_4$

Strongly Correlated Electrons 2022-08-10 v1 Materials Science

Abstract

The AA-site spinel NiRh2_2O4_4 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) and x-ray absorption spectroscopy (XAS) to characterize the local electronic structure of NiRh2_2O4_4. The RIXS data can be partly described by a single-ion model for tetrahedrally coordinated Ni2+^{2+} and indicates a tetragonal distortion Δt2 ⁣= ⁣70\Delta t_2\!=\!70 meV that splits the t2t_2 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 NiRh2_2O4_4. 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 NiRh2_2O4_4 and further demonstrate that covalency and lattice dynamics play essential roles in controlling the magnetic ground states of AA-site spinels.

Keywords

Cite

@article{arxiv.2205.12296,
  title  = {Electronic structure of the frustrated diamond lattice magnet NiRh$_2$O$_4$},
  author = {B. Zager and J. R. Chamorro and L. Ge and V. Bisogni and J. Pelliciari and J. Li and G. Fabbris and T. M. McQueen and M. Mourigal and K. W. Plumb},
  journal= {arXiv preprint arXiv:2205.12296},
  year   = {2022}
}