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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