skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Nature Communications
 [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)

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.

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
Citation Metrics:
Cited by: 23 works
Citation information provided by
Web of Science

References (66)

Control of the Electronic Properties and Resistive Switching in the New Series of Mott Insulators GaTa 4 Se 8– y Te y (0 ≤ y ≤ 6.5) journal May 2011
Valence Bond Glass on an fcc Lattice in the Double Perovskite Ba 2 YMoO 6 journal April 2010
Spin-singlet state formation in the cluster Mott insulator GaNb 4 S 8 studied by μ SR and NMR spectroscopy journal January 2010
Triplet and in-gap magnetic states in the ground state of the quantum frustrated fcc antiferromagnet Ba 2 YMoO 6 journal September 2011
Correlated Quantum Phenomena in the Strong Spin-Orbit Regime journal March 2014
Quantum spin liquid in the FCC lattice journal January 2003
Mott physics and band topology in materials with strong spin–orbit interaction journal March 2010
Colloquium: Hidden Order, Superconductivity, and Magnetism -- The Unsolved Case of URu2Si2 text January 2011
Voltage- and time-dependent valence state transition in cobalt oxide catalysts during the oxygen evolution reaction journal April 2020
Spin-orbital Entangled Molecular $j_{\rm eff}$ States in Lacunar Spinel Compounds text January 2014
Antiferromagnetic order and domains in Sr 3 Ir 2 O 7 probed by x-ray resonant scattering journal May 2012
Optical Conductivity Measurements of GaTa 4 Se 8 Under High Pressure: Evidence of a Bandwidth-Controlled Insulator-to-Metal Mott Transition journal January 2013
Correlated quantum phenomena in the strong spin-orbit regime text January 2013
Resonant inelastic x-ray scattering studies of elementary excitations journal June 2011
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models journal January 2009
Electric Pulse Induced Resistive Switching, Electronic Phase Separation, and Possible Superconductivity in a Mott insulator text January 2009
Observation of a $d$-wave gap in electron-doped Sr$_2$IrO$_4$ text January 2015
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study journal January 1998
Magnetic Field-Induced Transitions in the Mo4 Cluster Compounds GaMo4S8 and GaMo4Se8 Showing Heavy Fermion Behaviour journal August 1987
Spin-orbit coupling, strong correlation, and insulator-metal transitions: The J eff = 3 2 ferromagnetic Dirac-Mott insulator Ba 2 NaOsO 6 journal January 2015
Antiferromagnetic order and domains in Sr3Ir2O7 probed by x-ray resonant scattering text January 2012
Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4 journal March 2009
Colloquium : Hidden order, superconductivity, and magnetism: The unsolved case of URu 2 Si 2 journal November 2011
Itinerant electron magnetism in the Mo4 tetrahedral cluster compounds GaMo4S8, GaMo4Se8, and GaMo4Se4Te4 journal September 1983
A relativistic density functional formalism journal August 1979
Fermi arcs in a doped pseudospin-1/2 Heisenberg antiferromagnet journal June 2014
Ferromagnetism in the Mott Insulator Ba 2 NaOsO 6 journal July 2007
Observation of a d-wave gap in electron-doped Sr2IrO4 journal October 2015
Transition from Mott Insulator to Superconductor in G a N b 4 S e 8 and G a T a 4 S e 8 under High Pressure journal September 2004
Über die Streuung von Strahlung durch Atome journal February 1925
Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides A 2 IrO 3 journal July 2010
Magnetic ground state of Sr 2 IrO 4 and implications for second-harmonic generation journal August 2016
Direct Evidence for Dominant Bond-directional Interactions in a Honeycomb Lattice Iridate Na2IrO3 preprint January 2015
Dimensionality Driven Spin-Flop Transition in Layered Iridates text January 2012
Low-temperature series expansions for the FCC Ising antiferromagnet journal September 1981
Crystal and Electronic Structure of the Tetrahedral V4 Cluster Compounds GeV4Q8 (Q = S, Se) journal June 1998
Nouveaux chalcogénures et chalcohalogénures à clusters tétraédriques Nb4 ou Ta4 journal September 1984
Crystal Structures, Electronic Properties, and Pressure-Induced Superconductivity of the Tetrahedral Cluster Compounds GaNb 4 S 8 , GaNb 4 Se 8 , and GaTa 4 Se 8 journal June 2005
Electric-Pulse-driven Electronic Phase Separation, Insulator-Metal Transition, and Possible Superconductivity in a Mott Insulator journal July 2008
The Jahn-Teller effect and magnetism: transition metal compounds journal April 1982
The Jahn-Teller effect and magnetism: transition metal compounds [Effekt Yana - Tellera i magnetizm: soedineniya perekhodnykh metallov] journal January 1982
Elimination of the inner-shell lifetime broadening in x-ray-absorption spectroscopy journal November 1991
Variationally optimized atomic orbitals for large-scale electronic structures journal April 2003
Metallization of Mo-Cluster Compound Ga 0.5 Mo 2 S 4 at 38 GPa journal June 1990
Kitaev-Heisenberg models for iridates on the triangular, hyperkagome, kagome, fcc, and pyrochlore lattices journal January 2014
Frustrated magnetism in a Mott insulator based on a transition metal chalcogenide journal February 2016
First-Order Insulator-to-Metal Mott Transition in the Paramagnetic 3D System GaTa 4 Se 8 journal August 2014
Transition from Mott Insulator to Superconductor in $G a N b_ 4 S e_ 8$ and $G a T a_ 4 S e_ 8$ under High Pressure text January 2004
Robustness of Basal-Plane Antiferromagnetic Order and the J eff = 1 / 2 State in Single-Layer Iridate Spin-Orbit Mott Insulators journal March 2013
Spherical analyzers and monochromators for resonant inelastic hard X-ray scattering: a compilation of crystals and reflections journal November 2012
Thick-Restart Lanczos Method for Large Symmetric Eigenvalue Problems journal January 2000
Crystal Structures, Electronic Properties, and Pressure-Induced Superconductivity of the Tetrahedral Cluster Compounds GaNb4S8, GaNb4Se8, and GaTa4Se8. journal October 2005
Microscopic Study of a Spin-Orbit-Induced Mott Insulator in Ir Oxides journal November 2010
Resonant X-ray Diffraction Study of the Strongly Spin-Orbit-Coupled Mott Insulator CaIrO 3 journal May 2013
Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3 journal May 2015
Exotic phases induced by strong spin-orbit coupling in ordered double perovskites journal November 2010
Novel J eff = 1 / 2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr 2 IrO 4 journal August 2008
Twisted Hubbard Model for Sr 2 IrO 4 : Magnetism and Possible High Temperature Superconductivity journal March 2011
Magnetic Excitation Spectra of Sr 2 IrO 4 Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors journal April 2012
Monte Carlo Study of an Unconventional Superconducting Phase in Iridium Oxide J eff = 1 / 2 Mott Insulators Induced by Carrier Doping journal January 2013
Spin-liquid behavior in J eff = 1 2 triangular lattice compound Ba 3 IrTi 2 O 9 journal October 2012
Frustration-driven spin freezing in the S = 1 2 fcc perovskite Sr 2 MgReO 6 journal October 2003
Magnetic properties of the geometrically frustrated S = 1 2 antiferromagnets, La 2 LiMoO 6 and Ba 2 YMoO 6 , with the B-site ordered double perovskite structure: Evidence for a collective spin-singlet ground state journal June 2010
Dimensionality Driven Spin-Flop Transition in Layered Iridates journal July 2012
J eff = 1 2 Mott spin-orbit insulating state close to the cubic limit in Ca 4 IrO 6 journal February 2014
O ( N ) LDA + U electronic structure calculation method based on the nonorthogonal pseudoatomic orbital basis journal January 2006

Cited By (2)

Assessing exchange-correlation functional performance in the chalcogenide lacunar spinels Ga M 4 Q 8 ( M = Mo ,   V ,   Nb ,   Ta ; Q = S , Se ) journal September 2019
Ordering of hidden multipoles in spin-orbit entangled 5 d 1 Ta chlorides journal July 2019