Spin-Orbit Coupling Controlled J=3/2 Electronic Ground State in 5d3 Oxides

Taylor, A. E.; Calder, S.; Morrow, R.; Feng, H. L.; Upton, M. H.; Lumsden, M. D.; Yamaura, K.; Woodward, P. M.; Christianson, A. D.

doi:10.1103/PhysRevLett.118.207202

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

Journal Article · Tue May 16 00:00:00 EDT 2017 · Physical Review Letters

DOI:https://doi.org/10.1103/PhysRevLett.118.207202· OSTI ID:1362222

Taylor, A. E. ^[1]; Calder, S. ^[1]; Morrow, R. ^[2]; Feng, H. L. ^[3]; Upton, M. H. ^[4]; Lumsden, M. D. ^[1]; Yamaura, K. ^[3]; Woodward, P. M. ^[2]; Christianson, A. D. ^[5]

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)

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 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 5d³ case.

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Research Organization:: 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 Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

OSTI ID:: 1362222

Alternate ID(s):: OSTI ID: 1357315

Journal Information:: Physical Review Letters, Vol. 118, Issue 20; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 25 works

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Spin and orbital excitations through the metal-to-insulator transition in ${Cd}_{2} {Os}_{2} O_{7}$ probed with high-resolution resonant inelastic x-ray scattering Vale, J. G.; Calder, S.; Bogdanov, N. A. Physical Review B, Vol. 101, Issue 1 https://doi.org/10.1103/physrevb.101.014441	journal	January 2020
Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates Paramekanti, Arun; Singh, David J.; Yuan, Bo arXiv https://doi.org/10.48550/arxiv.1804.02006	text	January 2018
Octupolar order in d-orbital Mott insulators Paramekanti, Arun; Maharaj, Dalini D.; Gaulin, Bruce D. arXiv https://doi.org/10.48550/arxiv.1909.03089	text	January 2019

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