Quasimolecular electronic structure of the trimer iridate Ba4NbIr3O12

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • M. Magnaterra - , University of Cologne (Author)
  • A. Sandberg - , Stockholm University (Author)
  • H. Schilling - , University of Cologne (Author)
  • P. Warzanowski - , University of Cologne (Author)
  • L. Pätzold - , University of Cologne (Author)
  • E. Bergamasco - , University of Cologne (Author)
  • Ch J. Sahle - , European Synchrotron Radiation Facility (Author)
  • B. Detlefs - , European Synchrotron Radiation Facility (Author)
  • K. Ruotsalainen - , European Synchrotron Radiation Facility (Author)
  • M. Moretti Sala - , Polytechnic University of Milan (Author)
  • G. Monaco - , University of Padua (Author)
  • P. Becker - , University of Cologne (Author)
  • Q. Faure - , Université Paris-Saclay (Author)
  • G. S. Thakur - , Indian Institute of Science Education and Research, Berhampur, Max Planck Institute for Chemical Physics of Solids (Author)
  • M. Songvilay - , Université Grenoble Alpes (Author)
  • C. Felser - , Max Planck Institute for Chemical Physics of Solids (Author)
  • P. H.M. Van Loosdrecht - , University of Cologne (Author)
  • J. Van Den Brink - , Clusters of Excellence ct.qmat: Complexity and Topology in Quantum Matter, Chair of Solid State Theory, Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • M. Hermanns - , Stockholm University (Author)
  • M. Grüninger - , University of Cologne (Author)

Abstract

The insulating mixed-valent Ir+3.66 compound Ba4NbIr3O12 hosts two holes per Ir3O12 trimer unit. We address the electronic structure via resonant inelastic x-ray scattering (RIXS) at the Ir L3 edge and exact diagonalization. The holes occupy quasimolecular orbitals that are delocalized over a trimer. This gives rise to a rich intra-t2g excitation spectrum that extends from 0.5 eV to energies larger than 2 eV. Furthermore, it yields a strong modulation of the RIXS intensity as a function of the transferred momentum q. A clear fingerprint of the quasimolecular trimer character is the observation of two modulation periods, 2π/d and 2π/2d, where d and 2d denote the intratrimer Ir-Ir distances. We discuss how the specific modulation reflects the character of the wave function of an excited state. Our quantitative analysis shows that spin-orbit coupling λ of about 0.4 eV is decisive for the character of the electronic states, despite a large hopping ta1g of about 0.8 eV. The ground state of a single trimer is described very well by both holes occupying the bonding j=12 orbital, forming a vanishing quasimolecular moment with J=0.

Details

Original languageEnglish
Article number085122
Number of pages18
JournalPhysical Review B
Volume111
Issue number8
Publication statusPublished - 15 Feb 2025
Peer-reviewedYes