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

Jeong, Min Yong; Chang, Seo Hyoung; Kim, Beom Hyun; Sim, Jae -Hoon; Said, Ayman; Casa, Diego; Gog, Thomas; Janod, Etienne; Cario, Laurent; Yunoki, Seiji; Han, Myung Joon; Kim, Jungho

doi:10.1038/s41467-017-00841-9

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

Journal Article · 04 October 2017 · Nature Communications

DOI: https://doi.org/10.1038/s41467-017-00841-9 · OSTI ID:1413991

Jeong, Min Yong ^[1]; Chang, Seo Hyoung ^[2]; Kim, Beom Hyun ^[3]; Sim, Jae -Hoon ^[1]; Said, Ayman ^[4]; Casa, Diego ^[4]; Gog, Thomas ^[4]; Janod, Etienne ^[5]; Cario, Laurent ^[5]; Yunoki, Seiji ^[6]; Han, Myung Joon ^[1]; Kim, Jungho ^[4]

Korea Advanced Institute of Science and Technology, Daejeon (Korea)
Chung-Ang Univ., Seoul (Korea)
RIKEN, Saitama (Japan)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. de Nantes, Nantes cedex (France)
RIKEN, Saitama (Japan); RIKEN Center for Emergent Matter Science (CEMS), Saitama (Japan); RIKEN Advanced Institute for Computational Science (AICS), Hyogo (Japan)

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-rays scattering at the Ta L₃ and L₂ edges. In conclusion, we found that the excitations involving the J_eff = 1/2 molecular orbital were absent only at the Ta L₂ edge, manifesting the realization of the molecular J_eff = 3/2 ground state in GaTa₄Se₈.

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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; RIKEN; National Research Foundation of Korea (NRF); Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1413991

Journal Information:: Nature Communications, Vol. 8, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 26 works

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

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