Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates
Abstract
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)more »
- Authors:
-
- 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
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Natural Sciences and Engineering Research Council of Canada (NSERC)
- OSTI Identifier:
- 1454394
- Alternate Identifier(s):
- OSTI ID: 1441102; OSTI ID: 1462735
- Grant/Contract Number:
- AC05-00OR22725; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 97; Journal Issue: 23; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; electronic structure; magnetism; spin-orbit coupling
Citation Formats
Paramekanti, Arun, Singh, David J., Yuan, Bo, Casa, Diego, Said, Ayman, Kim, Young -June, and Christianson, Andrew D. Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates. United States: N. p., 2018.
Web. doi:10.1103/PhysRevB.97.235119.
Paramekanti, Arun, Singh, David J., Yuan, Bo, Casa, Diego, Said, Ayman, Kim, Young -June, & Christianson, Andrew D. Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates. United States. https://doi.org/10.1103/PhysRevB.97.235119
Paramekanti, Arun, Singh, David J., Yuan, Bo, Casa, Diego, Said, Ayman, Kim, Young -June, and Christianson, Andrew D. Mon .
"Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates". United States. https://doi.org/10.1103/PhysRevB.97.235119. https://www.osti.gov/servlets/purl/1454394.
@article{osti_1454394,
title = {Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates},
author = {Paramekanti, Arun and Singh, David J. and Yuan, Bo and Casa, Diego and Said, Ayman and Kim, Young -June and Christianson, Andrew D.},
abstractNote = {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.},
doi = {10.1103/PhysRevB.97.235119},
journal = {Physical Review B},
number = 23,
volume = 97,
place = {United States},
year = {Mon Jun 11 00:00:00 EDT 2018},
month = {Mon Jun 11 00:00:00 EDT 2018}
}
Web of Science
Figures / Tables:
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
Theory of resonant inelastic x-ray scattering in iridium oxide compounds: Probing spin-orbit-entangled ground states and excitations
journal, July 2011
- Ament, Luuk J. P.; Khaliullin, Giniyat; van den Brink, Jeroen
- Physical Review B, Vol. 84, Issue 2
Electronic structure and magnetism in Ru-based perovskites
journal, August 1997
- Mazin, I. I.; Singh, D. J.
- Physical Review B, Vol. 56, Issue 5
Ab initio analysis of the tight-binding parameters and magnetic interactions in Na IrO
journal, July 2013
- Foyevtsova, Kateryna; Jeschke, Harald O.; Mazin, I. I.
- Physical Review B, Vol. 88, Issue 3
Challenges in design of Kitaev materials: Magnetic interactions from competing energy scales
journal, June 2016
- Winter, Stephen M.; Li, Ying; Jeschke, Harald O.
- Physical Review B, Vol. 93, Issue 21
Orbital occupancies and the putative ground state in Ba IrO : A combined oxygen -edge XAS and RIXS study
journal, March 2014
- Moretti Sala, M.; Rossi, M.; Boseggia, S.
- Physical Review B, Vol. 89, Issue 12
Spin-Orbit Coupling Controlled Electronic Ground State in Oxides
journal, May 2017
- Taylor, A. E.; Calder, S.; Morrow, R.
- Physical Review Letters, Vol. 118, Issue 20
Correlated Quantum Phenomena in the Strong Spin-Orbit Regime
journal, March 2014
- Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek
- Annual Review of Condensed Matter Physics, Vol. 5, Issue 1
Magnetic nature of the 500 meV peak in observed with resonant inelastic x-ray scattering at the -edge
journal, February 2010
- Ellis, D. S.; Kim, Jungho; Hill, J. P.
- Physical Review B, Vol. 81, Issue 8
Diluted paramagnetic impurities in nonmagnetic
journal, October 2017
- Hammerath, F.; Sarkar, R.; Kamusella, S.
- Physical Review B, Vol. 96, Issue 16
Novel Magnetism of Ions in the Double Perovskite
journal, February 2014
- Cao, G.; Qi, T. F.; Li, L.
- Physical Review Letters, Vol. 112, Issue 5
Magnetic Excitation Spectra of Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors
journal, April 2012
- Kim, Jungho; Casa, D.; Upton, M. H.
- Physical Review Letters, Vol. 108, Issue 17
Ultrashort lifetime expansion for indirect resonant inelastic x-ray scattering
journal, March 2007
- Ament, Luuk J. P.; Forte, Filomena; van den Brink, Jeroen
- Physical Review B, Vol. 75, Issue 11
Phase Diagram and Quantum Order by Disorder in the Kitaev Honeycomb Magnet
journal, December 2015
- Rousochatzakis, Ioannis; Reuther, Johannes; Thomale, Ronny
- Physical Review X, Vol. 5, Issue 4
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
Resonant inelastic x-ray scattering operators for orbital systems
journal, August 2017
- Kim, B. J.; Khaliullin, Giniyat
- Physical Review B, Vol. 96, Issue 8
Frustrated fcc antiferromagnet : Structural characterization, magnetic properties, and neutron scattering studies
journal, February 2015
- Kermarrec, E.; Marjerrison, C. A.; Thompson, C. M.
- Physical Review B, Vol. 91, Issue 7
Unified theory of spiral magnetism in the harmonic-honeycomb iridates , and
journal, June 2015
- Kimchi, Itamar; Coldea, Radu; Vishwanath, Ashvin
- Physical Review B, Vol. 91, Issue 24
Topological crystalline metal in orthorhombic perovskite iridates
journal, March 2015
- Chen, Yige; Lu, Yuan-Ming; Kee, Hae-Young
- Nature Communications, Vol. 6, Issue 1
Resonant Inelastic X-Ray Scattering Response of the Kitaev Honeycomb Model
journal, September 2016
- Halász, Gábor B.; Perkins, Natalia B.; van den Brink, Jeroen
- Physical Review Letters, Vol. 117, Issue 12
Noncoplanar and Counterrotating Incommensurate Magnetic Order Stabilized by Kitaev Interactions in
journal, November 2014
- Biffin, A.; Johnson, R. D.; Kimchi, I.
- Physical Review Letters, Vol. 113, Issue 19
Exotic phases induced by strong spin-orbit coupling in ordered double perovskites
journal, November 2010
- Chen, Gang; Pereira, Rodrigo; Balents, Leon
- Physical Review B, Vol. 82, Issue 17
Theory of indirect resonant inelastic X-ray scattering
journal, December 2005
- van den Brink, Jeroen; van Veenendaal, Michel
- Journal of Physics and Chemistry of Solids, Vol. 66, Issue 12
Excitations in Manganites Probed by Resonant Inelastic X-Ray Scattering
journal, February 2005
- Grenier, S.; Hill, J. P.; Kiryukhin, V.
- Physical Review Letters, Vol. 94, Issue 4
First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA + U method
journal, January 1997
- Anisimov, Vladimir I.; Aryasetiawan, F.; Lichtenstein, A. I.
- Journal of Physics: Condensed Matter, Vol. 9, Issue 4, p. 767-808
Excitonic Magnetism in Van Vleck–type Mott Insulators
journal, November 2013
- Khaliullin, Giniyat
- Physical Review Letters, Vol. 111, Issue 19
Resonant Inelastic X-Ray Scattering Study of Charge Excitations in
journal, October 2002
- Kim, Y. J.; Hill, J. P.; Burns, C. A.
- Physical Review Letters, Vol. 89, Issue 17
: A spin-orbit assisted Mott insulator on a honeycomb lattice
journal, July 2014
- Plumb, K. W.; Clancy, J. P.; Sandilands, L. J.
- Physical Review B, Vol. 90, Issue 4
High-Energy Magnetic Excitations in the Cuprate Superconductor : Towards a Unified Description of Its Electronic and Magnetic Degrees of Freedom
journal, April 2013
- Dean, M. P. M.; James, A. J. A.; Springell, R. S.
- Physical Review Letters, Vol. 110, Issue 14
The theory of indirect resonant inelastic X-ray scattering on magnons
journal, October 2007
- van den Brink, J.
- Europhysics Letters (EPL), Vol. 80, Issue 4
Mixing of orbitals in and transition metal oxides
journal, February 2018
- Stamokostas, Georgios L.; Fiete, Gregory A.
- Physical Review B, Vol. 97, Issue 8
Interplay of spin-orbit coupling and hybridization in and
journal, November 2017
- Calder, S.; Singh, D. J.; Garlea, V. O.
- Physical Review B, Vol. 96, Issue 18
Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides
journal, July 2010
- Chaloupka, Jiří; Jackeli, George; Khaliullin, Giniyat
- Physical Review Letters, Vol. 105, Issue 2
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
Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate
journal, June 2014
- Modic, K. A.; Smidt, Tess E.; Kimchi, Itamar
- Nature Communications, Vol. 5, Issue 1
Magnetic excitations in probed by indirect resonant inelastic x-ray scattering
journal, April 2008
- Forte, Filomena; Ament, Luuk J. P.; van den Brink, Jeroen
- Physical Review B, Vol. 77, Issue 13
Doping-Induced Ferromagnetism and Possible Triplet Pairing in Mott Insulators
journal, January 2016
- Chaloupka, Jiří; Khaliullin, Giniyat
- Physical Review Letters, Vol. 116, Issue 1
Magnetic and calorimetric studies of double perovskites Ba 2 LnReO 6 (Ln = Y, Nd, Sm–Lu)
journal, January 2002
- Sasaki, Yoshinori; Doi, Yoshihiro; Hinatsu, Yukio
- J. Mater. Chem., Vol. 12, Issue 8
Spin-orbit coupling in ordered double perovskites
journal, September 2011
- Chen, Gang; Balents, Leon
- Physical Review B, Vol. 84, Issue 9
Unraveling Orbital Correlations with Magnetic Resonant Inelastic X-Ray Scattering
journal, September 2012
- Marra, Pasquale; Wohlfeld, Krzysztof; van den Brink, Jeroen
- Physical Review Letters, Vol. 109, Issue 11
Superconducting pairing in resonant inelastic x-ray scattering
journal, September 2016
- Shi, Yifei; Benjamin, David; Demler, Eugene
- Physical Review B, Vol. 94, Issue 9
Observation of heavy spin-orbit excitons propagating in a nonmagnetic background: The case of
journal, February 2018
- Kusch, M.; Katukuri, V. M.; Bogdanov, N. A.
- Physical Review B, Vol. 97, Issue 6
Determination of Hund's coupling in oxides using resonant inelastic x-ray scattering
journal, June 2017
- Yuan, Bo; Clancy, J. P.; Cook, A. M.
- Physical Review B, Vol. 95, Issue 23
Effective magnetic interactions in spin-orbit coupled Mott insulators
journal, January 2017
- Svoboda, Christopher; Randeria, Mohit; Trivedi, Nandini
- Physical Review B, Vol. 95, Issue 1
Novel Mott State Induced by Relativistic Spin-Orbit Coupling in
journal, August 2008
- Kim, B. J.; Jin, Hosub; Moon, S. J.
- Physical Review Letters, Vol. 101, Issue 7
Resonant inelastic x-ray scattering as a probe of band structure effects in cuprates
journal, October 2016
- Kanász-Nagy, M.; Shi, Y.; Klich, I.
- Physical Review B, Vol. 94, Issue 16
Magnetism out of antisite disorder in the compound
journal, October 2017
- Chen, Q.; Svoboda, C.; Zheng, Q.
- Physical Review B, Vol. 96, Issue 14
Magnetic excitations in a spin-orbit-coupled Mott insulator on the square lattice
journal, July 2014
- Akbari, Alireza; Khaliullin, Giniyat
- Physical Review B, Vol. 90, Issue 3
Hyperhoneycomb Iridate as a Platform for Kitaev Magnetism
journal, February 2015
- Takayama, T.; Kato, A.; Dinnebier, R.
- Physical Review Letters, Vol. 114, Issue 7
Novel magnetic state in Mott insulators
journal, February 2015
- Meetei, O. Nganba; Cole, William S.; Randeria, Mohit
- Physical Review B, Vol. 91, Issue 5
Generic Spin Model for the Honeycomb Iridates beyond the Kitaev Limit
journal, February 2014
- Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young
- Physical Review Letters, Vol. 112, Issue 7
Spiral order in the honeycomb iridate
journal, September 2014
- Reuther, Johannes; Thomale, Ronny; Rachel, Stephan
- Physical Review B, Vol. 90, Issue 10
Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates
journal, March 2012
- Singh, Yogesh; Manni, S.; Reuther, J.
- Physical Review Letters, Vol. 108, Issue 12
Correlation functions measured by indirect resonant inelastic X-ray scattering
journal, January 2006
- Brink, J. van den; Veenendaal, M. van
- Europhysics Letters (EPL), Vol. 73, Issue 1
: A Spin-Orbit Mott Insulator Beyond the Ground State
journal, April 2014
- Sala, M. Moretti; Ohgushi, K.; Al-Zein, A.
- Physical Review Letters, Vol. 112, Issue 17
Long-range magnetic order in the 5 d 2 double perovskite Ba 2 CaOsO 6 : comparison with spin-disordered Ba 2 YReO 6
journal, July 2014
- Thompson, C. M.; Carlo, J. P.; Flacau, R.
- Journal of Physics: Condensed Matter, Vol. 26, Issue 30
Evidence for a low-temperature magnetic ground state in double-perovskite iridates with ions
journal, August 2017
- Terzic, J.; Zheng, H.; Ye, Feng
- Physical Review B, Vol. 96, Issue 6
Three-band Hubbard model for : Topological insulator, zigzag antiferromagnet, and Kitaev-Heisenberg material
journal, September 2017
- Laubach, Manuel; Reuther, Johannes; Thomale, Ronny
- Physical Review B, Vol. 96, Issue 12
: A cubic double perovskite material with ions
journal, January 2016
- Dey, T.; Maljuk, A.; Efremov, D. V.
- Physical Review B, Vol. 93, Issue 1
Resonant Inelastic X-Ray Scattering as a Probe of the Phase and Excitations of the Order Parameter of Superconductors
journal, March 2013
- Marra, Pasquale; Sykora, Steffen; Wohlfeld, Krzysztof
- Physical Review Letters, Vol. 110, Issue 11
Breakdown of nonmagnetic state in iridate double perovskites: A first-principles study
journal, September 2015
- Bhowal, Sayantika; Baidya, Santu; Dasgupta, Indra
- Physical Review B, Vol. 92, Issue 12
Auxiliary fermion approach to the resonant inelastic x-ray scattering response in an underdoped cuprate
journal, October 2017
- Shi, Yifei; James, Andrew J. A.; Demler, Eugene
- Physical Review B, Vol. 96, Issue 15
Theoretical Demonstration of How the Dispersion of Magnetic Excitations in Cuprate Compounds can be Determined Using Resonant Inelastic X-Ray Scattering
journal, September 2009
- Ament, Luuk J. P.; Ghiringhelli, Giacomo; Sala, Marco Moretti
- Physical Review Letters, Vol. 103, Issue 11
Structure and magnetic properties of the geometrically frustrated double perovskites and
journal, February 2010
- Aharen, Tomoko; Greedan, John E.; Bridges, Craig A.
- Physical Review B, Vol. 81, Issue 6
Magnetic excitation spectrum of Na IrO probed with resonant inelastic x-ray scattering
journal, June 2013
- Gretarsson, H.; Clancy, J. P.; Singh, Yogesh
- Physical Review B, Vol. 87, Issue 22
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009
- Jackeli, G.; Khaliullin, G.
- Physical Review Letters, Vol. 102, Issue 1
Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3
journal, May 2015
- Hwan Chun, Sae; Kim, Jong-Woo; Kim, Jungho
- Nature Physics, Vol. 11, Issue 6
Is the ground state of 5 d 4 double-perovskite Iridate Ba 2 YIrO 6 magnetic or nonmagnetic?
journal, May 2018
- Gong, Hoshin; Kim, Kyoo; Kim, Beom Hyun
- Journal of Magnetism and Magnetic Materials, Vol. 454
Magnetic nature of the 500 meV peak in $\rm La_{2-x}Sr_{x}CuO_4$ observed with resonant inelastic x-ray scattering at the Cu $K$-edge
text, January 2010
- Ellis, D. S.; Kim, Jungho; Hill, J. P.
- arXiv
Unraveling Orbital Correlations via Magnetic Resonant Inelastic X-ray Scattering
text, January 2012
- Marra, Pasquale; Wohlfeld, Krzysztof; Brink, Jeroen van den
- arXiv
Correlated quantum phenomena in the strong spin-orbit regime
text, January 2013
- Witczak-Krempa, William; Chen, Gang; Kim, Yong Baek
- arXiv
Generic spin model for the honeycomb iridates beyond the Kitaev limit
text, January 2013
- Rau, Jeffrey G.; Lee, Eric Kin-Ho; Kee, Hae-Young
- arXiv
Topological Crystalline Metal in Orthorhombic Perovskite Iridates
text, January 2014
- Chen, Yige; Lu, Yuan-Ming; Kee, Hae-Young
- arXiv
Resonant inelastic x-ray scattering as a probe of band structure effects in cuprates
text, January 2015
- Kanász-Nagy, Márton; Shi, Yifei; Klich, Israel
- arXiv
Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales
text, January 2016
- Winter, Stephen M.; Li, Ying; Jeschke, Harald O.
- arXiv
Resonant inelastic X-ray scattering response of the Kitaev honeycomb model
text, January 2016
- Halász, Gábor B.; Perkins, Natalia B.; Brink, Jeroen van den
- arXiv
Resonant inelastic x-ray scattering operators for $t_{2g}$ orbital systems
text, January 2017
- Kim, B. J.; Khaliullin, Giniyat
- arXiv
Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6
text, January 2017
- Calder, S.; Singh, D. J.; Garlea, V. O.
- arXiv
Electronic structure and magnetism in Ru based perovskites
text, January 1997
- Mazin, I. I.; Singh, D. J.
- arXiv
Works referencing / citing this record:
Origin of magnetic excitation gap in double perovskite
journal, December 2018
- Taylor, A. E.; Morrow, R.; Lumsden, M. D.
- Physical Review B, Vol. 98, Issue 21
Octupolar order in d-orbital Mott insulators
text, January 2019
- Paramekanti, Arun; Maharaj, Dalini D.; Gaulin, Bruce D.
- arXiv
Figures / Tables found in this record: