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Title: Direct experimental observation of the molecular J eff=3/2 ground state in the lacunar spinel GaTa 4Se 8

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 GaTa 4Se 8 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 GaTa 4Se 8 by means of excitation spectra of resonant inelastic x-rays scattering at the Ta L 3 and L 2 edges. In conclusion, we found that the excitations involving the J eff = 1/2 molecular orbital were absent only at the Ta L 2 edge, manifesting the realization of the molecular J eff = 3/2 ground state in GaTa 4Se 8.
Authors:
 [1] ;  [2] ;  [3] ;  [1] ;  [4] ;  [4] ;  [4] ;  [5] ;  [5] ;  [6] ;  [1] ;  [4]
  1. Korea Advanced Institute of Science and Technology, Daejeon (Korea)
  2. Chung-Ang Univ., Seoul (Korea)
  3. RIKEN, Saitama (Japan)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Univ. de Nantes, Nantes cedex (France)
  6. RIKEN, Saitama (Japan); RIKEN Center for Emergent Matter Science (CEMS), Saitama (Japan); RIKEN Advanced Institute for Computational Science (AICS), Hyogo (Japan)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; RIKEN; National Research Foundation of Korea (NRF); Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Jeff=3/2; RIXS
OSTI Identifier:
1413991

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, and Kim, Jungho. Direct experimental observation of the molecular J eff=3/2 ground state in the lacunar spinel GaTa4Se8. United States: N. p., Web. doi:10.1038/s41467-017-00841-9.
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. Direct experimental observation of the molecular J eff=3/2 ground state in the lacunar spinel GaTa4Se8. United States. doi:10.1038/s41467-017-00841-9.
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, and Kim, Jungho. 2017. "Direct experimental observation of the molecular J eff=3/2 ground state in the lacunar spinel GaTa4Se8". United States. doi:10.1038/s41467-017-00841-9. https://www.osti.gov/servlets/purl/1413991.
@article{osti_1413991,
title = {Direct experimental observation of the molecular J eff=3/2 ground state in the lacunar spinel GaTa4Se8},
author = {Jeong, Min Yong and Chang, Seo Hyoung and Kim, Beom Hyun and Sim, Jae -Hoon and Said, Ayman and Casa, Diego and Gog, Thomas and Janod, Etienne and Cario, Laurent and Yunoki, Seiji and Han, Myung Joon and Kim, Jungho},
abstractNote = {Strong spin-orbit coupling lifts the degeneracy of t2g orbitals in 5d transition-metal systems, leaving a Kramers doublet and quartet with effective angular momentum of Jeff = 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 Jeff = 3/2 ground state. Experimental verification of its existence is an important first step to exploring the consequences of the Jeff = 3/2 state. Here, we report direct experimental evidence of the Jeff = 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 Jeff = 1/2 molecular orbital were absent only at the Ta L2 edge, manifesting the realization of the molecular Jeff = 3/2 ground state in GaTa4Se8.},
doi = {10.1038/s41467-017-00841-9},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {10}
}

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