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

Title: Interplay of spin-orbit coupling and hybridization in Ca 3 LiOsO 6 and Ca 3 LiRuO 6

Abstract

Here, the electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J = 3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the magnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin gap and ordered local moment is observed, however the magnetic structure, Néel temperature, and exchange interactions are unaltered. To explain this behavior it is necessary to include both spin-orbit coupling and hybridization, indicating the importance of an intermediate coupling approach when describing 5d oxides.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1];  [3];  [4]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Missouri, Columbia, MO (United States)
  3. Chinese Academy of Sciences (CAS), Beijing (China)
  4. National Institute for Materials Science, Ibaraki (Japan); Hokkaido Univ., Hokkaido (Japan)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1486965
Alternate Identifier(s):
OSTI ID: 1409870
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 96; Journal Issue: 18; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Calder, Stuart A., Singh, David J., Garlea, Vasile O., Lumsden, Mark D., Shi, Y. G., Yamaura, K., and Christianson, Andrew D. Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.96.184426.
Calder, Stuart A., Singh, David J., Garlea, Vasile O., Lumsden, Mark D., Shi, Y. G., Yamaura, K., & Christianson, Andrew D. Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6. United States. doi:10.1103/PhysRevB.96.184426.
Calder, Stuart A., Singh, David J., Garlea, Vasile O., Lumsden, Mark D., Shi, Y. G., Yamaura, K., and Christianson, Andrew D. Wed . "Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6". United States. doi:10.1103/PhysRevB.96.184426. https://www.osti.gov/servlets/purl/1486965.
@article{osti_1486965,
title = {Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6},
author = {Calder, Stuart A. and Singh, David J. and Garlea, Vasile O. and Lumsden, Mark D. and Shi, Y. G. and Yamaura, K. and Christianson, Andrew D.},
abstractNote = {Here, the electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J = 3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the magnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin gap and ordered local moment is observed, however the magnetic structure, Néel temperature, and exchange interactions are unaltered. To explain this behavior it is necessary to include both spin-orbit coupling and hybridization, indicating the importance of an intermediate coupling approach when describing 5d oxides.},
doi = {10.1103/PhysRevB.96.184426},
journal = {Physical Review B},
number = 18,
volume = 96,
place = {United States},
year = {2017},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 5 works
Citation information provided by
Web of Science

Figures / Tables:

FIG. 1 FIG. 1: (a) Neutron powder diffraction data (black) and model (red) for Ca3LiRuO6 at 4 K. Tick marks correspond to, from top to bottom, the crystal structural, magnetic structure and Al sample holder. Inset: intensity of magnetic reflection at 2θ=22°. (b) Ca3LiOsO6 and Ca3LiRuO6 form the hexagonal 2H-perovskite structure. Magneticmore » Os5+/Ru5+ ions (blue) are surrounded by six oxygen anions (red spheres). These octahedra are separated along the c-axis by Li+ cations. Ca2+ ions (grey spheres) provide the charge balance. (c) The magnetic structure and exchange interaction pathways are shown.« less

Save / Share:

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Comparative NMR studies on Ca 3 LiRuO 6 and Ca 3 NaRuO 6
journal, May 2016


Orbital magnetism in Cd 2 Os 2 O 7 studied by x-ray magnetic circular dichroism
journal, November 2011


Electronic structure and magnetism in Ru-based perovskites
journal, August 1997


Spin-Orbit Coupling Controlled J = 3 / 2 Electronic Ground State in 5 d 3 Oxides
journal, May 2017


MAGNDATA : towards a database of magnetic structures. I. The commensurate case
journal, September 2016

  • Gallego, Samuel V.; Perez-Mato, J. Manuel; Elcoro, Luis
  • Journal of Applied Crystallography, Vol. 49, Issue 5
  • DOI: 10.1107/S1600576716012863

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


Symmetry-Based Computational Tools for Magnetic Crystallography
journal, July 2015


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


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

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


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


Synthesis, crystal structure and magnetic properties of A3A′RuO6 (A = Ca, Sr; A′ = Li, Na)
journal, February 1997


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


Strong Correlations from Hund’s Coupling
journal, April 2013


Spin-orbit coupling control of anisotropy, ground state and frustration in 5d2 Sr2MgOsO6
journal, August 2016

  • Morrow, Ryan; Taylor, Alice E.; Singh, D. J.
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep32462

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


Linear spin wave theory for single-Q incommensurate magnetic structures
journal, March 2015


The high-resolution powder diffractometer at the high flux isotope reactor
journal, March 2010


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

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

Magnetostriction-driven ground-state stabilization in 2H perovskites
journal, October 2016


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

    Works referencing / citing this record:

    Neutron Instruments for Research in Coordination Chemistry: Neutron Instruments for Research in Coordination Chemistry
    journal, January 2019

    • Xue, Zi-Ling; Ramirez-Cuesta, Anibal J.; Brown, Craig M.
    • European Journal of Inorganic Chemistry, Vol. 2019, Issue 8
    • DOI: 10.1002/ejic.201801076

    Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates
    journal, June 2018


    Origin of magnetic excitation gap in double perovskite Sr 2 FeOsO 6
    journal, December 2018


      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.