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

Abstract

Entanglement of spin and orbital degrees of freedom drives the formation of novel quantum and topological physical states. Here we report resonant inelastic x-ray scattering measurements of the transition metal oxides Ca3LiOsO6 and Ba2YOsO6, which reveals a dramatic spitting of the t2g manifold. We invoke an intermediate coupling approach that incorporates both spin-orbit coupling and electron-electron interactions on an even footing and reveal that the ground state of 5d3-based compounds, which has remained elusive in previously applied models, is a novel spin-orbit entangled J=3/2 electronic ground state. This work reveals the hidden diversity of spin-orbit controlled ground states in 5d systems and introduces a new arena in the search for spin-orbit controlled phases of matter.

Authors:
; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF) - Directorate for Engineering - Center for Emergent Materials (CEM); Japan Society for the Promotion of Science (JSPS)
OSTI Identifier:
1389049
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
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

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. 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., and Christianson, A. D. Mon . "Spin-Orbit Coupling Controlled J=3/2 Electronic Ground State in 5d3 Oxides". United States. doi:10.1103/PhysRevLett.118.207202.
@article{osti_1389049,
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 = {Entanglement of spin and orbital degrees of freedom drives the formation of novel quantum and topological physical states. Here we report resonant inelastic x-ray scattering measurements of the transition metal oxides Ca3LiOsO6 and Ba2YOsO6, which reveals a dramatic spitting of the t2g manifold. We invoke an intermediate coupling approach that incorporates both spin-orbit coupling and electron-electron interactions on an even footing and reveal that the ground state of 5d3-based compounds, which has remained elusive in previously applied models, is a novel spin-orbit entangled J=3/2 electronic ground state. This work reveals the hidden diversity of spin-orbit controlled ground states in 5d systems and introduces a new arena in the search for spin-orbit controlled phases of matter.},
doi = {10.1103/PhysRevLett.118.207202},
journal = {Physical Review Letters},
issn = {0031-9007},
number = 20,
volume = 118,
place = {United States},
year = {2017},
month = {5}
}

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