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

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 5d 3 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+ 5d 3 ions is an unquenched J = 3/2 state. Resonant inelastic x-ray scattering (RIXS) in Ca3LiOsO6 and Ba 2YOsO 6 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 5d 3 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:
Grant/Contract Number:
AC05-00OR22725; AC02-06CH11357
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)
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)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
OSTI Identifier:
1362222
Alternate Identifier(s):
OSTI ID: 1357315

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., 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.. 2017. "Spin-Orbit Coupling Controlled J=3/2 Electronic Ground State in 5d3 Oxides". United States. doi: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 = {2017},
month = {5}
}