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Enhanced hybridization in the electronic ground state of the intercalated honeycomb iridate Ag3LiIr2O6

A. de la Torre1, B. Zager1, F. Bahrami2, M. DiScala1, J. R. Chamorro3,4, M. H. Upton5, G. Fabbris5, D. Haskel5, D. Casa5 et al.

T. M. McQueen3,4,6, F. Tafti2, and K. W. Plumb1,*

  • 1Department of Physics, Brown University, Providence, Rhode Island 02912, USA
  • 2Department of Physics, Boston College, Chestnut Hill, Massachusetts 02467, USA
  • 3Department of Chemistry, Johns Hopkins University, Baltimore, Maryland 21218, USA
  • 4Institute for Quantum Matter, Department of Physics and Astronomy, Johns Hopkins University, Baltimore, Maryland 21218, USA
  • 5Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, USA
  • 6Department of Materials Science and Engineering, Johns Hopkins University, Baltimore, Maryland 21218, USA

  • *Corresponding author: kemp_plumb@brown.edu

Phys. Rev. B 104, L100416 – Published 22 September, 2021

DOI: https://doi.org/10.1103/PhysRevB.104.L100416

Abstract

We use x-ray spectroscopy at the Ir L3/L2 absorption edge to study powder samples of the intercalated honeycomb magnet Ag3LiIr2O6. Based on x-ray absorption and resonant inelastic x-ray scattering measurements, and exact diagonalization calculations including nearest-neighbor Ir-Ir electron hopping integrals, we argue that the intercalation of Ag atoms results in a delocalized electronic structure with enhanced Ir-O hybridization, departing from the local relativistic jeff=1/2 state. We find that the relative orbital contribution to the magnetic moment is increased and the magnetization density is spatially extended and asymmetric in this hybridized state. Our results confirm the importance of metal-ligand hybridization in the magnetism of transition metal oxides and provide empirical guidance for understanding the collective magnetism in intercalated honeycomb iridates.

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