Charge ordering in Ir dimers in the ground state of Ba5AlIr2O11

Katukuri, Vamshi M.; Lu, Xingye; McNally, D. E.; Dantz, Marcus; Strocov, Vladimir N.; Sala, M. Moretti; Upton, M. H.; Terzic, J.; Cao, G.; Yazyev, Oleg V.; Schmitt, Thorsten

doi:10.1103/physrevb.105.075114

Charge ordering in Ir dimers in the ground state of Ba₅AlIr₂O₁₁

Journal Article · Sun Feb 06 23:00:00 EST 2022 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.105.075114· OSTI ID:1897912

^[1]; ^[2]; McNally, D. E. ^[3]; Dantz, Marcus ^[3]; Strocov, Vladimir N. ^[3]; Sala, M. Moretti ^[4]; Upton, M. H. ^[5]; Terzic, J. ^[6]; Cao, G. ^[6]; Yazyev, Oleg V. ^[1]; Schmitt, Thorsten ^[3]

Ecole Polytechnique Federale Lausanne (EPFL) (Switzerland)
Paul Scherrer Inst. (PSI), Villigen (Switzerland); Beijing Normal University (China)
Paul Scherrer Inst. (PSI), Villigen (Switzerland)
European Synchrotron Radiation Facility (ESRF), Grenoble (France); Polytechnic Univ. of Milan (Italy)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Univ. of Colorado, Boulder, CO (United States)

It has been well established experimentally that the interplay of electronic correlations and spin-orbit interactions in Ir⁴⁺ and Ir⁵⁺ oxides results in insulating J_eff = 1/2 and J_eff = 0 ground states, respectively. However, in compounds where the structural dimerization of iridium ions is favorable, the direct Ir d-d hybridization can be significant and takes a key role. Here, in this study, we investigate the effects of direct Ir d-d hybridization in comparison with electronic correlations and spin-orbit coupling in Ba₅AlIr₂O₁₁, a compound with Ir dimers. Using a combination of ab initio many-body wave-function quantum chemistry calculations and resonant inelastic x-ray scattering experiments, we elucidate the electronic structure of Ba₅AlIr₂O₁₁. We find excellent agreement between the calculated and the measured spin-orbit excitations. Contrary to expectations, the analysis of the many-body wave function shows that the two Ir (Ir⁴⁺ and Ir⁵⁺) ions in the Ir₂O₉ dimer unit in this compound preserve their local J_eff character close to 1/2 and 0, respectively. The local point group symmetry at each of the Ir ions plays an important role, significantly limiting the direct d-d hybridization. Our results emphasize that minute details in the local crystal field environment can lead to dramatic differences in the electronic states in iridates and 5d oxides in general.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; Swiss National Science Foundation (SNSF); National Natural Science Foundation of China (NSFC); European Commission

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1897912

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 7 Vol. 105; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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