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

Paramekanti, Arun; Singh, David J.; Yuan, Bo; Casa, Diego; Said, Ayman; Kim, Young -June; Christianson, Andrew D.

doi:10.1103/PhysRevB.97.235119

Title: Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates

Journal Article · Mon Jun 11 00:00:00 EDT 2018 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.97.235119· OSTI ID:1454394

Paramekanti, Arun ^[1]; Singh, David J. ^[2]; Yuan, Bo ^[3]; Casa, Diego ^[4]; Said, Ayman ^[4]; Kim, Young -June ^[3];

^[5]

Univ. of Toronto, Toronto, ON (Canada). Dept. of Physics; Canadian Institute for Advanced Research, Toronto, ON (Canada)
Univ. of Missouri, Columbia, MO (United States). Dept. of Physics and Astronomy
Univ. of Toronto, Toronto, ON (Canada). Dept. of Physics
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division and Neutron Scattering Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy

Motivated by RIXS experiments on a wide range of complex heavy oxides, including rhenates, osmates, and iridates, we discuss the theory of RIXS for site-localized t(2g) orbital systems with strong spin-orbit coupling. For such systems, we present exact diagonalization results for the spectrum at different electron fillings, showing that it accesses "single-particle" and "multiparticle" excitations. This leads to a simple picture for the energies and intensities of the RIXS spectra in Mott insulators such as double perovskites which feature highly localized electrons, and yields estimates of the spin-orbit coupling and Hund's coupling in correlated 5d oxides. We present new higher resolution RIXS data at the Re L-3 edge in Ba2YReO6 which finds a previously unresolved peak splitting, providing further confirmation of our theoretical predictions. Using ab initio electronic structure calculations on Ba2MReO6 (with M = Re, Os, Ir) we show that while the atomic limit yields a reasonable effective Hamiltonian description of the experimental observations, effects such as t(2g)-e(g) interactions and hybridization with oxygen are important. Our ab initio estimate for the strength of the intersite exchange coupling shows that, compared to the d(3) systems, the exchange is one or two orders of magnitude weaker in the d(2) and d(4) materials, which may partly explain the suppression of long-range magnetic order in the latter compounds. As a way to interpolate between the site-localized picture and our electronic structure band calculations, we discuss the spin-orbital levels of the MO6 cluster. This suggests a possible role for intracluster excitons in Ba2YIrO6 which may lead to a weak breakdown of the atomic J(eff) = 0 picture and to small magnetic moments.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Natural Sciences and Engineering Research Council of Canada (NSERC)

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

OSTI ID:: 1454394

Alternate ID(s):: OSTI ID: 1441102; OSTI ID: 1462735

Journal Information:: Physical Review B, Vol. 97, Issue 23; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 24 works

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