Spin-Orbit Coupling Controlled J=3/2 Electronic Ground State in 5d3 Oxides

Taylor, A. E.; Calder, S.; Morrow, R.; Feng, H. L.; Upton, M. H.; Lumsden, M. D.; Yamaura, K.; Woodward, P. M.; Christianson, A. D.

doi:10.1103/PhysRevLett.118.207202

Spin-Orbit Coupling Controlled $J = 3 / 2$ Electronic Ground State in $5 d^{3}$ Oxides

Journal Article · Tue May 16 00:00:00 EDT 2017 · Physical Review Letters

DOI:https://doi.org/10.1103/PhysRevLett.118.207202· OSTI ID:1362222

Taylor, A. E. ^[1]; Calder, S. ^[1]; Morrow, R. ^[2]; Feng, H. L. ^[3]; Upton, M. H. ^[4]; Lumsden, M. D. ^[1]; Yamaura, K. ^[3]; Woodward, P. M. ^[2]; Christianson, A. D. ^[5]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
The Ohio State Univ., Columbus, OH (United States)
National Inst. for Materials Science (NIMS), Tsukuba (Japan)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Spin-orbit entanglement in 5d-based transition metal oxides (TMOs) has been identified as a route to a host of unconventional physical states including quantum spin liquids, Weyl semimetals, and axion insulators. Yet despite intense interest, no clear rules have emerged for the treatment of spin-orbit coupling (SOC) in 5d TMOs outside of idealised LS or jj coupling paradigms. This is exemplified in 5d³ oxides in which an orbitally-quenched singlet ground state is anticipated, yet SOC is manifest in the observed magnetic properties. Here we solve this long-outstanding puzzle by revealing that the electronic ground state of Os5+ 5d³ ions is an unquenched J = 3/2 state. Resonant inelastic x-ray scattering (RIXS) in Ca3LiOsO6 and Ba₂YOsO₆ exposes a SOC-controlled splitting of the t_2g manifold. The results are successfully described using an intermediate-coupling framework in which oxygen hybridisation promotes the breakdown of the orbital singlet. This framework opens the door to realistic treatment of SOC across a range of 5d TMOs beyond the 5d³ case.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR); Spallation Neutron Source

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1362222

Alternate ID(s):: OSTI ID: 1357315
OSTI ID: 1389049

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 20 Vol. 118; ISSN 0031-9007; ISSN PRLTAO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (41)

Recent advances in magnetic structure determination by neutron powder diffraction Rodríguez-Carvajal, Juan Physica B: Condensed Matter, Vol. 192, Issue 1-2 https://doi.org/10.1016/0921-4526(93)90108-I	journal	October 1993
Crystal structure and magnetic ordering of novel perovskite-related barium osmate Ba11Os4O24 Wakeshima, Makoto; Hinatsu, Yukio Solid State Communications, Vol. 136, Issue 9-10 https://doi.org/10.1016/j.ssc.2005.09.025	journal	December 2005
Crystal Growth and Structure and Magnetic Properties of the 5d Oxide Ca ₃ LiOsO ₆ : Extended Superexchange Magnetic Interaction in Oxide Shi, Youguo; Guo, Yanfeng; Yu, Shan Journal of the American Chemical Society, Vol. 132, Issue 24 https://doi.org/10.1021/ja102606q	journal	June 2010
Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7 Calder, S.; Vale, J. G.; Bogdanov, N. A. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11651	journal	June 2016
Structural phase transitions and magnetic order in SrTcO3 Thorogood, Gordon J.; Avdeev, Maxim; Carter, Melody L. Dalton Transactions, Vol. 40, Issue 27 https://doi.org/10.1039/c1dt10445d	journal	January 2011
Magnetic Properties and Optical Absorption Spectrum of K ₂ ReCl ₆ Eisenstein, J. C. The Journal of Chemical Physics, Vol. 34, Issue 5 https://doi.org/10.1063/1.1701058	journal	May 1961
Optical Spectrum of Re ⁴⁺ in Single Crystals of K ₂ PtCl ₆ and Cs ₂ ZrCl ₆ at 4.2°K Dorain, Paul B.; Wheeler, Robert G. The Journal of Chemical Physics, Vol. 45, Issue 4 https://doi.org/10.1063/1.1727734	journal	August 1966
Momentum-resolved Resonant and Nonresonant Inelastic X-ray Scattering at the Advanced Photon Source Gog, T.; Seidler, G. T.; Casa, D. M. Synchrotron Radiation News, Vol. 22, Issue 6 https://doi.org/10.1080/08940880903397009	journal	November 2009
Effect of frustrations on magnetism in the Ru double perovskite Sr 2 YRuO 6 Kuz’min, E. V.; Ovchinnikov, S. G.; Singh, D. J. Physical Review B, Vol. 68, Issue 2 https://doi.org/10.1103/PhysRevB.68.024409	journal	July 2003
Sr 2 Cr Os O 6 : End point of a spin-polarized metal-insulator transition by 5 d band filling Krockenberger, Y.; Mogare, K.; Reehuis, M. Physical Review B, Vol. 75, Issue 2 https://doi.org/10.1103/PhysRevB.75.020404	journal	January 2007
Spin-orbit coupling in d 2 ordered double perovskites Chen, Gang; Balents, Leon Physical Review B, Vol. 84, Issue 9 https://doi.org/10.1103/PhysRevB.84.094420	journal	September 2011
Antiferromagnetic order and domains in Sr 3 Ir 2 O 7 probed by x-ray resonant scattering Boseggia, S.; Springell, R.; Walker, H. C. Physical Review B, Vol. 85, Issue 18 https://doi.org/10.1103/PhysRevB.85.184432	journal	May 2012
Magnetic structure determination of Ca 3 LiOsO 6 using neutron and x-ray scattering Calder, S.; Lumsden, M. D.; Garlea, V. O. Physical Review B, Vol. 86, Issue 5 https://doi.org/10.1103/PhysRevB.86.054403	journal	August 2012
Frustrated fcc antiferromagnet Ba 2 YOsO 6 : Structural characterization, magnetic properties, and neutron scattering studies Kermarrec, E.; Marjerrison, C. A.; Thompson, C. M. Physical Review B, Vol. 91, Issue 7 https://doi.org/10.1103/PhysRevB.91.075133	journal	February 2015
Magnetic order and electronic structure of the 5 d 3 double perovskite Sr 2 ScOsO 6 Taylor, A. E.; Morrow, R.; Singh, D. J. Physical Review B, Vol. 91, Issue 10 https://doi.org/10.1103/PhysRevB.91.100406	journal	March 2015
Electronic structure, local magnetism, and spin-orbit effects of Ir(IV)-, Ir(V)-, and Ir(VI)-based compounds Laguna-Marco, M. A.; Kayser, P.; Alonso, J. A. Physical Review B, Vol. 91, Issue 21 https://doi.org/10.1103/PhysRevB.91.214433	journal	June 2015
Fragility of ferromagnetic double exchange interactions and pressure tuning of magnetism in 3 d − 5 d double perovskite Sr 2 FeOsO 6 Veiga, L. S. I.; Fabbris, G.; van Veenendaal, M. Physical Review B, Vol. 91, Issue 23 https://doi.org/10.1103/PhysRevB.91.235135	journal	June 2015
Ba 2 YIrO 6 : A cubic double perovskite material with Ir 5 + ions Dey, T.; Maljuk, A.; Efremov, D. V. Physical Review B, Vol. 93, Issue 1 https://doi.org/10.1103/PhysRevB.93.014434	journal	January 2016
Spin-orbit coupling controlled ground state in Sr 2 ScOsO 6 Taylor, A. E.; Morrow, R.; Fishman, R. S. Physical Review B, Vol. 93, Issue 22 https://doi.org/10.1103/PhysRevB.93.220408	journal	June 2016
Lifshitz transition driven by spin fluctuations and spin-orbit renormalization in NaOsO 3 Kim, Bongjae; Liu, Peitao; Ergönenc, Zeynep Physical Review B, Vol. 94, Issue 24 https://doi.org/10.1103/PhysRevB.94.241113	journal	December 2016
Strongly gapped spin-wave excitation in the insulating phase of NaOsO 3 Calder, S.; Vale, J. G.; Bogdanov, N. Physical Review B, Vol. 95, Issue 2 https://doi.org/10.1103/PhysRevB.95.020413	journal	January 2017
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models Jackeli, G.; Khaliullin, G. Physical Review Letters, Vol. 102, Issue 1 https://doi.org/10.1103/PhysRevLett.102.017205	journal	January 2009
High Temperature Magnetic Ordering in the 4 d Perovskite SrTcO 3 Rodriguez, Efrain E.; Poineau, Frédéric; Llobet, Anna Physical Review Letters, Vol. 106, Issue 6 https://doi.org/10.1103/PhysRevLett.106.067201	journal	February 2011
Magnetic Excitation Spectra of Sr 2 IrO 4 Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors Kim, Jungho; Casa, D.; Upton, M. H. Physical Review Letters, Vol. 108, Issue 17 https://doi.org/10.1103/PhysRevLett.108.177003	journal	April 2012
Magnetically Driven Metal-Insulator Transition in NaOsO 3 Calder, S.; Garlea, V. O.; McMorrow, D. F. Physical Review Letters, Vol. 108, Issue 25 https://doi.org/10.1103/PhysRevLett.108.257209	journal	June 2012
Testing the Validity of the Strong Spin-Orbit-Coupling Limit for Octahedrally Coordinated Iridate Compounds in a Model System Sr 3 CuIrO 6 Liu, X.; Katukuri, Vamshi M.; Hozoi, L. Physical Review Letters, Vol. 109, Issue 15 https://doi.org/10.1103/PhysRevLett.109.157401	journal	October 2012
Theory of High T c Ferrimagnetism in a Multiorbital Mott Insulator Meetei, O. Nganba; Erten, Onur; Randeria, Mohit Physical Review Letters, Vol. 110, Issue 8 https://doi.org/10.1103/PhysRevLett.110.087203	journal	February 2013
Novel Magnetism of Ir 5 + ( 5 d 4 ) Ions in the Double Perovskite Sr 2 YIrO 6 Cao, G.; Qi, T. F.; Li, L. Physical Review Letters, Vol. 112, Issue 5 https://doi.org/10.1103/PhysRevLett.112.056402	journal	February 2014
CaIrO 3 : A Spin-Orbit Mott Insulator Beyond the j eff = 1 / 2 Ground State Sala, M. Moretti; Ohgushi, K.; Al-Zein, A. Physical Review Letters, Vol. 112, Issue 17 https://doi.org/10.1103/PhysRevLett.112.176402	journal	April 2014
Resonant inelastic x-ray scattering studies of elementary excitations Ament, Luuk J. P.; van Veenendaal, Michel; Devereaux, Thomas P. Reviews of Modern Physics, Vol. 83, Issue 2 https://doi.org/10.1103/RevModPhys.83.705	journal	June 2011
EXPGUI , a graphical user interface for GSAS Toby, Brian H. Journal of Applied Crystallography, Vol. 34, Issue 2 https://doi.org/10.1107/S0021889801002242	journal	April 2001
Ordered double perovskites – a group-theoretical analysis Howard, Christopher J.; Kennedy, Brendan J.; Woodward, Patrick M. Acta Crystallographica Section B Structural Science, Vol. 59, Issue 4 https://doi.org/10.1107/S0108768103010073	journal	July 2003
Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4 Kim, B. J.; Ohsumi, H.; Komesu, T. Science, Vol. 323, Issue 5919 https://doi.org/10.1126/science.1167106	journal	March 2009
Magnetic Properties of the Pd and Pt Group Transition Metal Complexes Kamimura, Hiroshi; Koide, Shoichiro; Sekiyama, Hisao Journal of the Physical Society of Japan, Vol. 15, Issue 7 https://doi.org/10.1143/JPSJ.15.1264	journal	July 1960
Electron Correlation and Ferromagnetism of Transition Metals Kanamori, Junjiro Progress of Theoretical Physics, Vol. 30, Issue 3 https://doi.org/10.1143/PTP.30.275	journal	September 1963
Strong Correlations from Hund’s Coupling Georges, Antoine; Medici, Luca de'; Mravlje, Jernej Annual Review of Condensed Matter Physics, Vol. 4, Issue 1 https://doi.org/10.1146/annurev-conmatphys-020911-125045	journal	April 2013
Correlated Quantum Phenomena in the Strong Spin-Orbit Regime Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek Annual Review of Condensed Matter Physics, Vol. 5, Issue 1 https://doi.org/10.1146/annurev-conmatphys-020911-125138	journal	March 2014
Correlated quantum phenomena in the strong spin-orbit regime Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek arXiv https://doi.org/10.48550/arxiv.1305.2193	text	January 2013
Lifshitz transition driven by spin fluctuations and spin-orbit renormalization in NaOsO$_3$ Kim, Bongjae; Liu, Peitao; Ergönenc, Zeynep arXiv https://doi.org/10.48550/arxiv.1601.03310	text	January 2016
Strongly Gapped Spin-Wave Excitation in the Insulating Phase of NaOsO3 Calder, S.; Vale, J. G.; Bogdanov, N. arXiv https://doi.org/10.48550/arxiv.1608.08477	text	January 2016
Effect of Spin–Orbit Interaction on (4 d ) ³ - and (5 d ) ³ -Based Transition-Metal Oxides Matsuura, Hiroyasu; Miyake, Kazumasa Journal of the Physical Society of Japan, Vol. 82, Issue 7 https://doi.org/10.7566/JPSJ.82.073703	journal	July 2013

Cited By (9)

Spin-orbit coupling induced magnetic anisotropy and large spin wave gap in NaOsO ₃ Singh, Avinash; Mohapatra, Shubhajyoti; Bhandari, Churna Journal of Physics Communications, Vol. 2, Issue 11 https://doi.org/10.1088/2399-6528/aaef6a	journal	November 2018
Ground state in the novel dimer iridate B a 13 I r 6 O 30 with I r 6 + ( 5 d 3 ) ions Zhao, Hengdi; Ye, Feng; Zheng, Hao Physical Review B, Vol. 100, Issue 6 https://doi.org/10.1103/physrevb.100.064418	journal	August 2019
Spin and orbital excitations through the metal-to-insulator transition in Cd 2 Os 2 O 7 probed with high-resolution resonant inelastic x-ray scattering Vale, J. G.; Calder, S.; Bogdanov, N. A. Physical Review B, Vol. 101, Issue 1 https://doi.org/10.1103/physrevb.101.014441	journal	January 2020
Octupolar order in d -orbital Mott insulators Paramekanti, A.; Maharaj, D. D.; Gaulin, B. D. Physical Review B, Vol. 101, Issue 5 https://doi.org/10.1103/physrevb.101.054439	journal	February 2020
Hybridized orbital states in spin-orbit coupled 3 d − 5 d double perovskites studied by x-ray absorption spectroscopy Lee, Min-Cheol; Lee, Sanghyun; Won, C. J. Physical Review B, Vol. 97, Issue 12 https://doi.org/10.1103/physrevb.97.125123	journal	March 2018
Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates Paramekanti, Arun; Singh, David J.; Yuan, Bo Physical Review B, Vol. 97, Issue 23 https://doi.org/10.1103/physrevb.97.235119	journal	June 2018
Origin of magnetic excitation gap in double perovskite Sr 2 FeOsO 6 Taylor, A. E.; Morrow, R.; Lumsden, M. D. Physical Review B, Vol. 98, Issue 21 https://doi.org/10.1103/physrevb.98.214422	journal	December 2018
Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates Paramekanti, Arun; Singh, David J.; Yuan, Bo arXiv https://doi.org/10.48550/arxiv.1804.02006	text	January 2018
Octupolar order in d-orbital Mott insulators Paramekanti, Arun; Maharaj, Dalini D.; Gaulin, Bruce D. arXiv https://doi.org/10.48550/arxiv.1909.03089	text	January 2019

Similar Records

Spin-Orbit Coupling Controlled

J = 3 / 2

Electronic Ground State in

5 d^{3}

Oxides

Journal Article · Mon May 01 00:00:00 EDT 2017 · Physical Review Letters · OSTI ID:1389049

Evidence for a low-temperature magnetic ground state in double-perovskite iridates with

I r^{5 +} (5 d^{4})

ions

Journal Article · Tue Aug 29 00:00:00 EDT 2017 · Physical Review B · OSTI ID:1471893

Spin gaps in the ordered states of

{La}_{2} Li X O_{6} (X = Ru, Os)

and their relation to the distortion of the cubic double perovskite structure in

4 d^{3}

and

5 d^{3}

magnets

Journal Article · Fri Sep 28 00:00:00 EDT 2018 · Physical Review B · OSTI ID:1493992

Related Subjects

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS