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Direct experimental observation of the molecular J eff = 3/2 ground state in the lacunar spinel GaTa4Se8

Min Yong Jeong, Seo Hyoung Chang, Beom Hyun Kim, Jae-Hoon Sim, Ayman Said, Diego Casa, Thomas Gog, Etienne Janod, Laurent Cario, Seiji Yunoki, Myung Joon Han () and Jungho Kim ()
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Min Yong Jeong: Korea Advanced Institute of Science and Technology
Seo Hyoung Chang: Chung-Ang University
Beom Hyun Kim: Computational Condensed Matter Physics Laboratory, RIKEN, Wako
Jae-Hoon Sim: Korea Advanced Institute of Science and Technology
Ayman Said: Advanced Photon Source, Argonne National Laboratory
Diego Casa: Advanced Photon Source, Argonne National Laboratory
Thomas Gog: Advanced Photon Source, Argonne National Laboratory
Etienne Janod: Institut des Matériaux Jean Rouxel (IMN), Université de Nantes, CNRS
Laurent Cario: Institut des Matériaux Jean Rouxel (IMN), Université de Nantes, CNRS
Seiji Yunoki: Computational Condensed Matter Physics Laboratory, RIKEN, Wako
Myung Joon Han: Korea Advanced Institute of Science and Technology
Jungho Kim: Advanced Photon Source, Argonne National Laboratory

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: Abstract Strong spin–orbit coupling lifts the degeneracy of t 2g orbitals in 5d transition-metal systems, leaving a Kramers doublet and quartet with effective angular momentum of J eff = 1/2 and 3/2, respectively. These spin–orbit entangled states can host exotic quantum phases such as topological Mott state, unconventional superconductivity, and quantum spin liquid. The lacunar spinel GaTa4Se8 was theoretically predicted to form the molecular J eff = 3/2 ground state. Experimental verification of its existence is an important first step to exploring the consequences of the J eff = 3/2 state. Here, we report direct experimental evidence of the J eff = 3/2 state in GaTa4Se8 by means of excitation spectra of resonant inelastic X-ray scattering at the Ta L3 and L2 edges. We find that the excitations involving the J eff = 1/2 molecular orbital are absent only at the Ta L2 edge, manifesting the realization of the molecular J eff = 3/2 ground state in GaTa4Se8.

Date: 2017
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DOI: 10.1038/s41467-017-00841-9

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