Covalency-driven collapse of strong spin-orbit coupling in face-sharing iridium octahedra

Mai Ye, Heung Sik Kim, Jae Wook Kim, Choong Jae Won, Kristjan Haule, David Vanderbilt, Sang Wook Cheong, G. Blumberg

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

We report ab initio density functional theory calculation and Raman scattering results to explore the electronic structure of Ba5CuIr3O12 single crystals. This insulating iridate, consisting of face-sharing IrO6 octahedra forming quasi-one-dimensional chains, cannot be described by the local jeff=1/2 moment picture commonly adopted for discussing the electronic and magnetic properties of iridate compounds with IrO6 octahedra. The shorter Ir-Ir distance in the face-sharing geometry, compared to corner- or edge-sharing structures, leads to strong covalency between neighboring Ir. Then, this strong covalency results in the formation of molecular orbitals (MOs) at each Ir trimer as the low-energy electronic degree of freedom. The theoretically predicted three-peak structure in the joint density of states, a distinct indication of deviation from the jeff=1/2 picture, is verified by observing the three-peak structure in the electronic excitation spectrum by Raman scattering.

Original languageEnglish (US)
Article number201105
JournalPhysical Review B
Volume98
Issue number20
DOIs
StatePublished - Nov 9 2018

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Iridium
iridium
Raman scattering
Orbits
orbits
Molecular orbitals
electronics
Electronic properties
Raman spectra
Electronic structure
Density functional theory
Magnetic properties
Single crystals
trimers
Geometry
molecular orbitals
indication
degrees of freedom
density functional theory
electronic structure

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

Cite this

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title = "Covalency-driven collapse of strong spin-orbit coupling in face-sharing iridium octahedra",
abstract = "We report ab initio density functional theory calculation and Raman scattering results to explore the electronic structure of Ba5CuIr3O12 single crystals. This insulating iridate, consisting of face-sharing IrO6 octahedra forming quasi-one-dimensional chains, cannot be described by the local jeff=1/2 moment picture commonly adopted for discussing the electronic and magnetic properties of iridate compounds with IrO6 octahedra. The shorter Ir-Ir distance in the face-sharing geometry, compared to corner- or edge-sharing structures, leads to strong covalency between neighboring Ir. Then, this strong covalency results in the formation of molecular orbitals (MOs) at each Ir trimer as the low-energy electronic degree of freedom. The theoretically predicted three-peak structure in the joint density of states, a distinct indication of deviation from the jeff=1/2 picture, is verified by observing the three-peak structure in the electronic excitation spectrum by Raman scattering.",
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Covalency-driven collapse of strong spin-orbit coupling in face-sharing iridium octahedra. / Ye, Mai; Kim, Heung Sik; Kim, Jae Wook; Won, Choong Jae; Haule, Kristjan; Vanderbilt, David; Cheong, Sang Wook; Blumberg, G.

In: Physical Review B, Vol. 98, No. 20, 201105, 09.11.2018.

Research output: Contribution to journalArticle

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AU - Kim, Heung Sik

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AU - Won, Choong Jae

AU - Haule, Kristjan

AU - Vanderbilt, David

AU - Cheong, Sang Wook

AU - Blumberg, G.

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AB - We report ab initio density functional theory calculation and Raman scattering results to explore the electronic structure of Ba5CuIr3O12 single crystals. This insulating iridate, consisting of face-sharing IrO6 octahedra forming quasi-one-dimensional chains, cannot be described by the local jeff=1/2 moment picture commonly adopted for discussing the electronic and magnetic properties of iridate compounds with IrO6 octahedra. The shorter Ir-Ir distance in the face-sharing geometry, compared to corner- or edge-sharing structures, leads to strong covalency between neighboring Ir. Then, this strong covalency results in the formation of molecular orbitals (MOs) at each Ir trimer as the low-energy electronic degree of freedom. The theoretically predicted three-peak structure in the joint density of states, a distinct indication of deviation from the jeff=1/2 picture, is verified by observing the three-peak structure in the electronic excitation spectrum by Raman scattering.

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