Spin-Orbit Coupling Controlled Electronic Ground State in 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:
-
- 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)
- 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}
}
Web of Science
Works referenced in this record:
Fragility of ferromagnetic double exchange interactions and pressure tuning of magnetism in double perovskite
journal, June 2015
- Veiga, L. S. I.; Fabbris, G.; van Veenendaal, M.
- Physical Review B, Vol. 91, Issue 23
Magnetically Driven Metal-Insulator Transition in
journal, June 2012
- Calder, S.; Garlea, V. O.; McMorrow, D. F.
- Physical Review Letters, Vol. 108, Issue 25
Effect of frustrations on magnetism in the Ru double perovskite
journal, July 2003
- Kuz’min, E. V.; Ovchinnikov, S. G.; Singh, D. J.
- Physical Review B, Vol. 68, Issue 2
Electronic structure, local magnetism, and spin-orbit effects of Ir(IV)-, Ir(V)-, and Ir(VI)-based compounds
journal, June 2015
- Laguna-Marco, M. A.; Kayser, P.; Alonso, J. A.
- Physical Review B, Vol. 91, Issue 21
: End point of a spin-polarized metal-insulator transition by band filling
journal, January 2007
- Krockenberger, Y.; Mogare, K.; Reehuis, M.
- Physical Review B, Vol. 75, Issue 2
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
EXPGUI , a graphical user interface for GSAS
journal, April 2001
- Toby, Brian H.
- Journal of Applied Crystallography, Vol. 34, Issue 2
Correlated Quantum Phenomena in the Strong Spin-Orbit Regime
journal, March 2014
- Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek
- Annual Review of Condensed Matter Physics, Vol. 5, Issue 1
Novel Magnetism of Ions in the Double Perovskite
journal, February 2014
- Cao, G.; Qi, T. F.; Li, L.
- Physical Review Letters, Vol. 112, Issue 5
Lifshitz transition driven by spin fluctuations and spin-orbit renormalization in
journal, December 2016
- Kim, Bongjae; Liu, Peitao; Ergönenc, Zeynep
- Physical Review B, Vol. 94, Issue 24
Antiferromagnetic order and domains in Sr Ir O probed by x-ray resonant scattering
journal, May 2012
- Boseggia, S.; Springell, R.; Walker, H. C.
- Physical Review B, Vol. 85, Issue 18
Magnetic Excitation Spectra of Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors
journal, April 2012
- Kim, Jungho; Casa, D.; Upton, M. H.
- Physical Review Letters, Vol. 108, Issue 17
Theory of High Ferrimagnetism in a Multiorbital Mott Insulator
journal, February 2013
- Meetei, O. Nganba; Erten, Onur; Randeria, Mohit
- Physical Review Letters, Vol. 110, Issue 8
Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993
- Rodríguez-Carvajal, Juan
- Physica B: Condensed Matter, Vol. 192, Issue 1-2
Magnetic order and electronic structure of the double perovskite
journal, March 2015
- Taylor, A. E.; Morrow, R.; Singh, D. J.
- Physical Review B, Vol. 91, Issue 10
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
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
Frustrated fcc antiferromagnet : Structural characterization, magnetic properties, and neutron scattering studies
journal, February 2015
- Kermarrec, E.; Marjerrison, C. A.; Thompson, C. M.
- Physical Review B, Vol. 91, Issue 7
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
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
Crystal structure and magnetic ordering of novel perovskite-related barium osmate Ba11Os4O24
journal, December 2005
- Wakeshima, Makoto; Hinatsu, Yukio
- Solid State Communications, Vol. 136, Issue 9-10
: A Spin-Orbit Mott Insulator Beyond the Ground State
journal, April 2014
- Sala, M. Moretti; Ohgushi, K.; Al-Zein, A.
- Physical Review Letters, Vol. 112, Issue 17
Electron Correlation and Ferromagnetism of Transition Metals
journal, September 1963
- Kanamori, Junjiro
- Progress of Theoretical Physics, Vol. 30, Issue 3
Spin-orbit coupling controlled ground state in
journal, June 2016
- Taylor, A. E.; Morrow, R.; Fishman, R. S.
- Physical Review B, Vol. 93, Issue 22
Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4
journal, March 2009
- Kim, B. J.; Ohsumi, H.; Komesu, T.
- Science, Vol. 323, Issue 5919
Strong Correlations from Hund’s Coupling
journal, April 2013
- Georges, Antoine; Medici, Luca de'; Mravlje, Jernej
- Annual Review of Condensed Matter Physics, Vol. 4, Issue 1
: A cubic double perovskite material with ions
journal, January 2016
- Dey, T.; Maljuk, A.; Efremov, D. V.
- Physical Review B, Vol. 93, Issue 1
Magnetic structure determination of Ca LiOsO using neutron and x-ray scattering
journal, August 2012
- Calder, S.; Lumsden, M. D.; Garlea, V. O.
- Physical Review B, Vol. 86, Issue 5
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
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
Testing the Validity of the Strong Spin-Orbit-Coupling Limit for Octahedrally Coordinated Iridate Compounds in a Model System
journal, October 2012
- Liu, X.; Katukuri, Vamshi M.; Hozoi, L.
- Physical Review Letters, Vol. 109, Issue 15
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009
- Jackeli, G.; Khaliullin, G.
- Physical Review Letters, Vol. 102, Issue 1
Momentum-resolved Resonant and Nonresonant Inelastic X-ray Scattering at the Advanced Photon Source
journal, November 2009
- Gog, T.; Seidler, G. T.; Casa, D. M.
- Synchrotron Radiation News, Vol. 22, Issue 6
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
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
High Temperature Magnetic Ordering in the Perovskite
journal, February 2011
- Rodriguez, Efrain E.; Poineau, Frédéric; Llobet, Anna
- Physical Review Letters, Vol. 106, Issue 6
Strongly gapped spin-wave excitation in the insulating phase of
journal, January 2017
- Calder, S.; Vale, J. G.; Bogdanov, N.
- Physical Review B, Vol. 95, Issue 2
Spin-orbit coupling in ordered double perovskites
journal, September 2011
- Chen, Gang; Balents, Leon
- Physical Review B, Vol. 84, Issue 9
Correlated quantum phenomena in the strong spin-orbit regime
text, January 2013
- Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek
- arXiv
Lifshitz transition driven by spin fluctuations and spin-orbit renormalization in NaOsO$_3$
text, January 2016
- Kim, Bongjae; Liu, Peitao; Ergönenc, Zeynep
- arXiv
Strongly Gapped Spin-Wave Excitation in the Insulating Phase of NaOsO3
text, January 2016
- Calder, S.; Vale, J. G.; Bogdanov, N.
- arXiv
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
Ground state in the novel dimer iridate with ions
journal, August 2019
- Zhao, Hengdi; Ye, Feng; Zheng, Hao
- Physical Review B, Vol. 100, Issue 6
Spin and orbital excitations through the metal-to-insulator transition in probed with high-resolution resonant inelastic x-ray scattering
journal, January 2020
- Vale, J. G.; Calder, S.; Bogdanov, N. A.
- Physical Review B, Vol. 101, Issue 1
Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates
text, January 2018
- Paramekanti, Arun; Singh, David J.; Yuan, Bo
- arXiv
Octupolar order in d-orbital Mott insulators
text, January 2019
- Paramekanti, Arun; Maharaj, Dalini D.; Gaulin, Bruce D.
- arXiv