J$_{\mathrm{eff}}=$1/2 Mott spin-orbit insulating state close to the cubic limit in Ca$_{4}$IrO$_{6}$

ORAL

Abstract

The J$_{\mathrm{eff}}=$1/2 Mott spin-orbit insulating state is manifested in systems with large cubic crystal field splitting and spin-orbit coupling that are comparable to the on-site Coulomb interaction, U. 5d transition metal oxides host parameters in this regime and recently strong evidence for this state in Sr$_{2}$IrO$_{4}$, and additional iridates, has been presented. All the candidates, however, have distorted octahedra, such as the elongation along the c-axis in Sr$_{2}$IrO$_{4}$, and consequently a non-cubic local crystal field environment. Consequently the materials form a mixed J$_{\mathrm{eff}}=$1/2,3/2 ground state. The lack of a material with an unmixed J$_{\mathrm{eff}}=$1/2 has impacted the development and testing of robust models of this novel insulating and magnetic state. We present neutron diffraction, resonant x-ray scattering and DFT calculations that not only reveal Ca$_{4}$IrO$_{6}$ is a new candidate J$_{\mathrm{eff}}=$1/2 material with long-range magnetic order, but furthermore resides close to the required cubic limit. Both our experimental and theoretical investigation indicate Ca$_{4}$IrO$_{6}$ is uniquely positioned to act as a canonical system to investigate of the J$_{\mathrm{eff}}=$1/2 state.

*This research was supported by the Scientific User Facilities Division and the Materials Sciences and Engineering Division, Office of Basic Energy Sciences, U.S. Department of Energy.

Authors

  • S. Calder

    • Oak Ridge National Lab
  • G.-X. Cao

    • Oak Ridge National Lab
  • Satoshi Okamoto

    • Oak Ridge National Lab
    • Oak Ridge National Laboratory
  • Jong-Woo Kim

    • Argonne National Laboratory
  • Valentino Cooper

    • Oak Ridge National Lab
    • Oak Ridge National Laboratory
    • Oak Ridge National Lab, Oak Ridge, TN
  • Zheng Gai

    • Oak Ridge National Lab
    • Oak Ridge National Laboratory
  • Brian Sales

    • Oak Ridge National Lab
    • Oak Ridge National Laboratory
  • M.D. Lumsden

    • Oak Ridge National Lab
    • Quantum Condensed Matter Division, Oak Ridge National Laboratory
  • David Mandrus

    • Oak Ridge Natl Lab
    • Department of Materials Science and Engineering, the University of Tennessee, Knoxville, TN 37996, USA
    • Oak Ridge National Lab
    • Univ of Tennessee
    • University of Tennessee and Oak Ridge National Laboratory
    • Univ of Tennessee Knoxville
    • University of Tennessee, Oak Ridge National Laboratory
  • A.D. Christianson

    • Oak Ridge National Lab
    • Oak Ridge National Laboratory
    • Quantum Condensed Matter Division, Oak Ridge National Laboratory