Spin-orbit-entangled state of Ba2CaOsO6 studied by O K-edge resonant inelastic X-ray scattering and Raman spectroscopy

Abstract Transition-metal ions with 5d 2 electronic configuration in a cubic crystal field are prone to have a vanishing dipolar magnetic moment but finite higher-order multipolar moments, and they are expected to exhibit exotic physical properties. Through an investigation using resonant inelastic...

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Main Authors: J. Okamoto, G. Shibata, Yu. S. Ponosov, H. Hayashi, K. Yamaura, H. Y. Huang, A. Singh, C. T. Chen, A. Tanaka, S. V. Streltsov, D. J. Huang, A. Fujimori
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Language:English
Published: Nature Portfolio 2025-04-01
Series:npj Quantum Materials
Online Access:https://doi.org/10.1038/s41535-025-00757-4
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author J. Okamoto
G. Shibata
Yu. S. Ponosov
H. Hayashi
K. Yamaura
H. Y. Huang
A. Singh
C. T. Chen
A. Tanaka
S. V. Streltsov
D. J. Huang
A. Fujimori
author_facet J. Okamoto
G. Shibata
Yu. S. Ponosov
H. Hayashi
K. Yamaura
H. Y. Huang
A. Singh
C. T. Chen
A. Tanaka
S. V. Streltsov
D. J. Huang
A. Fujimori
author_sort J. Okamoto
collection DOAJ
description Abstract Transition-metal ions with 5d 2 electronic configuration in a cubic crystal field are prone to have a vanishing dipolar magnetic moment but finite higher-order multipolar moments, and they are expected to exhibit exotic physical properties. Through an investigation using resonant inelastic X-ray scattering (RIXS), Raman spectroscopy, and theoretical ligand-field (LF) multiplet and ab initio calculations, we fully characterized the local electronic structure of Ba2CaOsO6, particularly, the crystal-field symmetry of the 5d 2 electrons in this anomalous material. The low-energy multiplet excitations from RIXS at the oxygen K edge and Raman-active phonons both show no splitting. These findings are consistent with the ground state of Os ions dominated by magnetic octupoles. Obtained parameters pave the way for further realistic microscopic studies of this highly unusual class of materials, advancing our understanding of spin-orbit physics in systems with higher-order multipoles.
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institution OA Journals
issn 2397-4648
language English
publishDate 2025-04-01
publisher Nature Portfolio
record_format Article
series npj Quantum Materials
spelling doaj-art-a6c1c333c1cc459494f0e6b471c62e2e2025-08-20T02:19:57ZengNature Portfolionpj Quantum Materials2397-46482025-04-011011810.1038/s41535-025-00757-4Spin-orbit-entangled state of Ba2CaOsO6 studied by O K-edge resonant inelastic X-ray scattering and Raman spectroscopyJ. Okamoto0G. Shibata1Yu. S. Ponosov2H. Hayashi3K. Yamaura4H. Y. Huang5A. Singh6C. T. Chen7A. Tanaka8S. V. Streltsov9D. J. Huang10A. Fujimori11National Synchrotron Radiation Research CenterMaterials Sciences Research Center, Japan Atomic Energy AgencyInstitute of Metal PhysicsResearch Center for Materials Nanoarchitectonics (MANA), National Institute for Materials ScienceResearch Center for Materials Nanoarchitectonics (MANA), National Institute for Materials ScienceNational Synchrotron Radiation Research CenterNational Synchrotron Radiation Research CenterNational Synchrotron Radiation Research CenterGraduate School of Advanced Science and Engineering, Hiroshima UniversityInstitute of Metal PhysicsNational Synchrotron Radiation Research CenterNational Synchrotron Radiation Research CenterAbstract Transition-metal ions with 5d 2 electronic configuration in a cubic crystal field are prone to have a vanishing dipolar magnetic moment but finite higher-order multipolar moments, and they are expected to exhibit exotic physical properties. Through an investigation using resonant inelastic X-ray scattering (RIXS), Raman spectroscopy, and theoretical ligand-field (LF) multiplet and ab initio calculations, we fully characterized the local electronic structure of Ba2CaOsO6, particularly, the crystal-field symmetry of the 5d 2 electrons in this anomalous material. The low-energy multiplet excitations from RIXS at the oxygen K edge and Raman-active phonons both show no splitting. These findings are consistent with the ground state of Os ions dominated by magnetic octupoles. Obtained parameters pave the way for further realistic microscopic studies of this highly unusual class of materials, advancing our understanding of spin-orbit physics in systems with higher-order multipoles.https://doi.org/10.1038/s41535-025-00757-4
spellingShingle J. Okamoto
G. Shibata
Yu. S. Ponosov
H. Hayashi
K. Yamaura
H. Y. Huang
A. Singh
C. T. Chen
A. Tanaka
S. V. Streltsov
D. J. Huang
A. Fujimori
Spin-orbit-entangled state of Ba2CaOsO6 studied by O K-edge resonant inelastic X-ray scattering and Raman spectroscopy
npj Quantum Materials
title Spin-orbit-entangled state of Ba2CaOsO6 studied by O K-edge resonant inelastic X-ray scattering and Raman spectroscopy
title_full Spin-orbit-entangled state of Ba2CaOsO6 studied by O K-edge resonant inelastic X-ray scattering and Raman spectroscopy
title_fullStr Spin-orbit-entangled state of Ba2CaOsO6 studied by O K-edge resonant inelastic X-ray scattering and Raman spectroscopy
title_full_unstemmed Spin-orbit-entangled state of Ba2CaOsO6 studied by O K-edge resonant inelastic X-ray scattering and Raman spectroscopy
title_short Spin-orbit-entangled state of Ba2CaOsO6 studied by O K-edge resonant inelastic X-ray scattering and Raman spectroscopy
title_sort spin orbit entangled state of ba2caoso6 studied by o k edge resonant inelastic x ray scattering and raman spectroscopy
url https://doi.org/10.1038/s41535-025-00757-4
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