DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Abstract

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 t2g 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.

Authors:
 [1];  [1];  [2];  [3];  [4];  [1];  [3];  [2];  [5]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. The Ohio State Univ., Columbus, OH (United States)
  3. National Inst. for Materials Science (NIMS), Tsukuba (Japan)
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1362222
Alternate Identifier(s):
OSTI ID: 1357315
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 118; Journal Issue: 20; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Taylor, A. E., Calder, S., Morrow, R., Feng, H. L., Upton, M. H., Lumsden, M. D., Yamaura, K., Woodward, P. M., and Christianson, A. D. Spin-Orbit Coupling Controlled J=3/2 Electronic Ground State in 5d3 Oxides. United States: N. p., 2017. Web. doi:10.1103/PhysRevLett.118.207202.
Taylor, A. E., Calder, S., Morrow, R., Feng, H. L., Upton, M. H., Lumsden, M. D., Yamaura, K., Woodward, P. M., & Christianson, A. D. Spin-Orbit Coupling Controlled J=3/2 Electronic Ground State in 5d3 Oxides. United States. https://doi.org/10.1103/PhysRevLett.118.207202
Taylor, A. E., Calder, S., Morrow, R., Feng, H. L., Upton, M. H., Lumsden, M. D., Yamaura, K., Woodward, P. M., and Christianson, A. D. Tue . "Spin-Orbit Coupling Controlled J=3/2 Electronic Ground State in 5d3 Oxides". United States. https://doi.org/10.1103/PhysRevLett.118.207202. https://www.osti.gov/servlets/purl/1362222.
@article{osti_1362222,
title = {Spin-Orbit Coupling Controlled J=3/2 Electronic Ground State in 5d3 Oxides},
author = {Taylor, A. E. and Calder, S. and Morrow, R. and Feng, H. L. and Upton, M. H. and Lumsden, M. D. and Yamaura, K. and Woodward, P. M. and Christianson, A. D.},
abstractNote = {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 t2g 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.},
doi = {10.1103/PhysRevLett.118.207202},
journal = {Physical Review Letters},
number = 20,
volume = 118,
place = {United States},
year = {Tue May 16 00:00:00 EDT 2017},
month = {Tue May 16 00:00:00 EDT 2017}
}

Journal Article:

Citation Metrics:
Cited by: 25 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Fragility of ferromagnetic double exchange interactions and pressure tuning of magnetism in 3 d 5 d double perovskite Sr 2 FeOsO 6
journal, June 2015


Magnetically Driven Metal-Insulator Transition in NaOsO 3
journal, June 2012


Effect of frustrations on magnetism in the Ru double perovskite Sr 2 YRuO 6
journal, July 2003


Electronic structure, local magnetism, and spin-orbit effects of Ir(IV)-, Ir(V)-, and Ir(VI)-based compounds
journal, June 2015


Sr 2 Cr Os O 6 : End point of a spin-polarized metal-insulator transition by 5 d band filling
journal, January 2007


Structural phase transitions and magnetic order in SrTcO3
journal, January 2011

  • Thorogood, Gordon J.; Avdeev, Maxim; Carter, Melody L.
  • Dalton Transactions, Vol. 40, Issue 27
  • DOI: 10.1039/c1dt10445d

EXPGUI , a graphical user interface for GSAS
journal, April 2001


Correlated Quantum Phenomena in the Strong Spin-Orbit Regime
journal, March 2014


Novel Magnetism of Ir 5 + ( 5 d 4 ) Ions in the Double Perovskite Sr 2 YIrO 6
journal, February 2014


Lifshitz transition driven by spin fluctuations and spin-orbit renormalization in NaOsO 3
journal, December 2016


Antiferromagnetic order and domains in Sr 3 Ir 2 O 7 probed by x-ray resonant scattering
journal, May 2012


Theory of High T c Ferrimagnetism in a Multiorbital Mott Insulator
journal, February 2013


Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993


Magnetic order and electronic structure of the 5 d 3 double perovskite Sr 2 ScOsO 6
journal, March 2015


Resonant inelastic x-ray scattering studies of elementary excitations
journal, June 2011

  • Ament, Luuk J. P.; van Veenendaal, Michel; Devereaux, Thomas P.
  • Reviews of Modern Physics, Vol. 83, Issue 2
  • DOI: 10.1103/RevModPhys.83.705

Optical Spectrum of Re 4+ in Single Crystals of K 2 PtCl 6 and Cs 2 ZrCl 6 at 4.2°K
journal, August 1966

  • Dorain, Paul B.; Wheeler, Robert G.
  • The Journal of Chemical Physics, Vol. 45, Issue 4
  • DOI: 10.1063/1.1727734

Frustrated fcc antiferromagnet Ba 2 YOsO 6 : Structural characterization, magnetic properties, and neutron scattering studies
journal, February 2015


Effect of Spin–Orbit Interaction on (4 d ) 3 - and (5 d ) 3 -Based Transition-Metal Oxides
journal, July 2013

  • Matsuura, Hiroyasu; Miyake, Kazumasa
  • Journal of the Physical Society of Japan, Vol. 82, Issue 7
  • DOI: 10.7566/JPSJ.82.073703

Ordered double perovskites – a group-theoretical analysis
journal, July 2003

  • Howard, Christopher J.; Kennedy, Brendan J.; Woodward, Patrick M.
  • Acta Crystallographica Section B Structural Science, Vol. 59, Issue 4
  • DOI: 10.1107/S0108768103010073

Crystal structure and magnetic ordering of novel perovskite-related barium osmate Ba11Os4O24
journal, December 2005


CaIrO 3 : A Spin-Orbit Mott Insulator Beyond the j eff = 1 / 2 Ground State
journal, April 2014


Electron Correlation and Ferromagnetism of Transition Metals
journal, September 1963

  • Kanamori, Junjiro
  • Progress of Theoretical Physics, Vol. 30, Issue 3
  • DOI: 10.1143/PTP.30.275

Spin-orbit coupling controlled ground state in Sr 2 ScOsO 6
journal, June 2016


Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4
journal, March 2009


Strong Correlations from Hund’s Coupling
journal, April 2013


Ba 2 YIrO 6 : A cubic double perovskite material with Ir 5 + ions
journal, January 2016


Magnetic structure determination of Ca 3 LiOsO 6 using neutron and x-ray scattering
journal, August 2012


Magnetic Properties of the Pd and Pt Group Transition Metal Complexes
journal, July 1960

  • Kamimura, Hiroshi; Koide, Shoichiro; Sekiyama, Hisao
  • Journal of the Physical Society of Japan, Vol. 15, Issue 7
  • DOI: 10.1143/JPSJ.15.1264

Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7
journal, June 2016

  • Calder, S.; Vale, J. G.; Bogdanov, N. A.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11651

Testing the Validity of the Strong Spin-Orbit-Coupling Limit for Octahedrally Coordinated Iridate Compounds in a Model System Sr 3 CuIrO 6
journal, October 2012


Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009


Momentum-resolved Resonant and Nonresonant Inelastic X-ray Scattering at the Advanced Photon Source
journal, November 2009


Magnetic Properties and Optical Absorption Spectrum of K 2 ReCl 6
journal, May 1961

  • Eisenstein, J. C.
  • The Journal of Chemical Physics, Vol. 34, Issue 5
  • DOI: 10.1063/1.1701058

Crystal Growth and Structure and Magnetic Properties of the 5d Oxide Ca 3 LiOsO 6 : Extended Superexchange Magnetic Interaction in Oxide
journal, June 2010

  • Shi, Youguo; Guo, Yanfeng; Yu, Shan
  • Journal of the American Chemical Society, Vol. 132, Issue 24
  • DOI: 10.1021/ja102606q

High Temperature Magnetic Ordering in the 4 d Perovskite SrTcO 3
journal, February 2011


Strongly gapped spin-wave excitation in the insulating phase of NaOsO 3
journal, January 2017


Spin-orbit coupling in d 2 ordered double perovskites
journal, September 2011


Correlated quantum phenomena in the strong spin-orbit regime
text, January 2013


Lifshitz transition driven by spin fluctuations and spin-orbit renormalization in NaOsO$_3$
text, January 2016


Strongly Gapped Spin-Wave Excitation in the Insulating Phase of NaOsO3
text, January 2016


Works referencing / citing this record:

Spin-orbit coupling induced magnetic anisotropy and large spin wave gap in NaOsO 3
journal, November 2018

  • Singh, Avinash; Mohapatra, Shubhajyoti; Bhandari, Churna
  • Journal of Physics Communications, Vol. 2, Issue 11
  • DOI: 10.1088/2399-6528/aaef6a

Ground state in the novel dimer iridate B a 13 I r 6 O 30 with I r 6 + ( 5 d 3 ) ions
journal, August 2019


Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates
text, January 2018


Octupolar order in d-orbital Mott insulators
text, January 2019