Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7

Calder, Stuart A; Vale, James G.; Bogdanov, Nikolay; Liu, Xeurong; Donnerer, Christian; Upton, Mary; Casa, Diego; Ayman, Said; Lumsden, M. D.; Zhao, Zhiying; Yan, J. -Q.; Mandrus, David; Satoshi, Nishimoto; Van den Brink, Jeroen; Hill, John P; McMorrow, D. F.; Christianson, Andrew D

doi:10.1038/ncomms11651

Title: Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd₂Os₂O₇

Abstract

Here, much consideration has been given to the role of spin-orbit coupling (SOC) in 5d oxides, particularly on the formation of novel electronic states and manifested metal-insulator transitions (MITs). SOC plays a dominant role in 5d⁵ iridates (Ir⁴⁺), undergoing MITs both concurrent (pyrochlores) and separated (perovskites) from the onset of magnetic order. However, the role of SOC for other 5d configurations is less clear. For example, 5d³ (Os⁵⁺) systems are expected to have an orbital singlet with reduced effective SOC. The pyrochlore Cd₂Os₂O₇ nonetheless exhibits a MIT entwined with magnetic order phenomenologically similar to pyrochlore iridates. Here, we resolve the magnetic structure in Cd₂Os₂O₇ with neutron diffraction and then via resonant inelastic X-ray scattering determine the salient electronic and magnetic energy scales controlling the MIT. In particular, SOC plays a subtle role in creating the electronic ground state but drives the magnetic order and emergence of a multiple spin-flip magnetic excitation.

Authors:

Calder, Stuart A ^[1]; Vale, James G. ^[2]; Bogdanov, Nikolay ^[3]; Liu, Xeurong ^[4]; Donnerer, Christian ^[5]; Upton, Mary ^[6]; Casa, Diego ^[6]; Ayman, Said ^[7]; Lumsden, M. D. ^[6]; Zhao, Zhiying ^[8]; Yan, J. -Q. ^[8]; Mandrus, David ^[8]; Satoshi, Nishimoto ^[9]; Van den Brink, Jeroen ^[9]; Hill, John P ^[10]; McMorrow, D. F. ^[5]; Christianson, Andrew D ^[11]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
Univ. College London (UCL), London (United Kingdom). London Centre for Nanotechnology
Leibniz Inst. for Solid State and Materials Research (IFW), Dresden (Germany)
Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed matter physics and materials science Dept.; Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics. Beijing National Lab. for Condensed Matter Physics (BNLCP-CAS)
Univ. College London (UCL), London (United Kingdom). London Centre for Nanotechnology
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Argonne National Laboratory (ANL), Advanced Photon Source (APS)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Leibniz Inst. for Solid State and Materials Research (IFW), Dresden (Germany); Technische Univ. Dresden (Germany)
Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy

Publication Date:: Tue Jun 07 00:00:00 EDT 2016

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Engineering and Physical Sciences Research Council (EPSRC); German Research Foundation (DFG); Ministry of Science and Technology of the People's Republic of China (MOST)

OSTI Identifier:: 1338574

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357; AC02-98CH10886; 2015CB921302; XDB07020200

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 7; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Spintronics; Magnetic properties and materials; Excited states

Citation Formats


                    Calder, Stuart A, Vale, James G., Bogdanov, Nikolay, Liu, Xeurong, Donnerer, Christian, Upton, Mary, Casa, Diego, Ayman, Said, Lumsden, M. D., Zhao, Zhiying, Yan, J. -Q., Mandrus, David, Satoshi, Nishimoto, Van den Brink, Jeroen, Hill, John P, McMorrow, D. F., and Christianson, Andrew D. Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7.  United States: N. p., 2016. 
Web.  doi:10.1038/ncomms11651.

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                    Calder, Stuart A, Vale, James G., Bogdanov, Nikolay, Liu, Xeurong, Donnerer, Christian, Upton, Mary, Casa, Diego, Ayman, Said, Lumsden, M. D., Zhao, Zhiying, Yan, J. -Q., Mandrus, David, Satoshi, Nishimoto, Van den Brink, Jeroen, Hill, John P, McMorrow, D. F., & Christianson, Andrew D. Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7.  United States.  https://doi.org/10.1038/ncomms11651

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                    Calder, Stuart A, Vale, James G., Bogdanov, Nikolay, Liu, Xeurong, Donnerer, Christian, Upton, Mary, Casa, Diego, Ayman, Said, Lumsden, M. D., Zhao, Zhiying, Yan, J. -Q., Mandrus, David, Satoshi, Nishimoto, Van den Brink, Jeroen, Hill, John P, McMorrow, D. F., and Christianson, Andrew D. Tue .  
"Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7".  United States.  https://doi.org/10.1038/ncomms11651.  https://www.osti.gov/servlets/purl/1338574.

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@article{osti_1338574,

  title        = {Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7},

  author       = {Calder, Stuart A and Vale, James G. and Bogdanov, Nikolay and Liu, Xeurong and Donnerer, Christian and Upton, Mary and Casa, Diego and Ayman, Said and Lumsden, M. D. and Zhao, Zhiying and Yan, J. -Q. and Mandrus, David and Satoshi, Nishimoto and Van den Brink, Jeroen and Hill, John P and McMorrow, D. F. and Christianson, Andrew D},

  abstractNote = {Here, much consideration has been given to the role of spin-orbit coupling (SOC) in 5d oxides, particularly on the formation of novel electronic states and manifested metal-insulator transitions (MITs). SOC plays a dominant role in 5d5 iridates (Ir4+), undergoing MITs both concurrent (pyrochlores) and separated (perovskites) from the onset of magnetic order. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (Os5+) systems are expected to have an orbital singlet with reduced effective SOC. The pyrochlore Cd2Os2O7 nonetheless exhibits a MIT entwined with magnetic order phenomenologically similar to pyrochlore iridates. Here, we resolve the magnetic structure in Cd2Os2O7 with neutron diffraction and then via resonant inelastic X-ray scattering determine the salient electronic and magnetic energy scales controlling the MIT. In particular, SOC plays a subtle role in creating the electronic ground state but drives the magnetic order and emergence of a multiple spin-flip magnetic excitation.},

  doi          = {10.1038/ncomms11651},

  journal      = {Nature Communications},

  number       = ,

  volume       = 7,

  place        = {United States},

  year         = {Tue Jun 07 00:00:00 EDT 2016},

  month        = {Tue Jun 07 00:00:00 EDT 2016}

}

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Title: Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7

Abstract

Citation Formats

Mott physics and band topology in materials with strong spin–orbit interaction journal, March 2010

Novel J eff = 1 / 2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr 2 IrO 4 journal, August 2008

Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4 journal, March 2009

Topological semimetal and Fermi-arc surface states in the electronic structure of pyrochlore iridates journal, May 2011

Correlated Quantum Phenomena in the Strong Spin-Orbit Regime journal, March 2014

Noncollinear Magnetism and Spin-Orbit Coupling in 5 d Pyrochlore Oxide Cd 2 Os 2 O 7 journal, June 2012

Tetrahedral Magnetic Order and the Metal-Insulator Transition in the Pyrochlore Lattice of Cd 2 Os 2 O 7 journal, June 2012

Continuous metal-insulator transition in the pyrochlore Cd 2 Os 2 O 7 journal, April 2001

Searching for the Slater transition in the pyrochlore Cd 2 Os 2 O 7 with infrared spectroscopy journal, July 2002

Orbital magnetism in Cd 2 Os 2 O 7 studied by x-ray magnetic circular dichroism journal, November 2011

Magnetic Effects and the Hartree-Fock Equation journal, May 1951

Anisotropy-Tuned Magnetic Order in Pyrochlore Iridates journal, June 2015

Determination of long-range all-in-all-out ordering of Ir 4 + moments in a pyrochlore iridate Eu 2 Ir 2 O 7 by resonant x-ray diffraction journal, March 2013

Magnetic Field-Induced Insulator-Semimetal Transition in a Pyrochlore Nd 2 Ir 2 O 7 journal, July 2015

Magnetic Excitation Spectra of Sr 2 IrO 4 Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors journal, April 2012

Large Spin-Wave Energy Gap in the Bilayer Iridate Sr 3 Ir 2 O 7 : Evidence for Enhanced Dipolar Interactions Near the Mott Metal-Insulator Transition journal, October 2012

CaIrO 3 : A Spin-Orbit Mott Insulator Beyond the j eff = 1 / 2 Ground State journal, April 2014

Testing the Validity of the Strong Spin-Orbit-Coupling Limit for Octahedrally Coordinated Iridate Compounds in a Model System Sr 3 CuIrO 6 journal, October 2012

Crystal-Field Splitting and Correlation Effect on the Electronic Structure of A 2 IrO 3 journal, February 2013

Excitonic quasiparticles in a spin–orbit Mott insulator journal, July 2014

Magnetic order and electronic structure of the 5 d 3 double perovskite Sr 2 ScOsO 6 journal, March 2015

Magnetic State of Pyrochlore Cd 2 Os 2 O 7 Emerging from Strong Competition of Ligand Distortions and Longer-Range Crystalline Anisotropy journal, March 2013

Strong Correlations from Hund’s Coupling journal, April 2013

Resonant inelastic x-ray scattering studies of elementary excitations journal, June 2011

The high-resolution powder diffractometer at the high flux isotope reactor journal, March 2010

A new protocol for the determination of magnetic structures using simulated annealing and representational analysis (SARAh) journal, March 2000

Momentum-resolved Resonant and Nonresonant Inelastic X-ray Scattering at the Advanced Photon Source journal, November 2009

Excitonic quasiparticles in a spin–orbit Mott insulator journal, July 2014

Longer-range lattice anisotropy strongly competing with spin-orbit interactions in pyrochlore iridates journal, March 2014

Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4 journal, March 2009

[OsF 6 ] x − : Molecular Models for Spin-Orbit Entangled Phenomena journal, July 2017

Neutron Instruments for Research in Coordination Chemistry: Neutron Instruments for Research in Coordination Chemistry journal, January 2019

Possible Origin of the Absence of Magnetic Order in LiOsO 3 : Spin–Orbit Coupling Controlled Ground State journal, September 2018

Strain‐Induced Slater Transition in Polar Metal LiOsO 3 journal, May 2019

Ferromagnetism above 1000 K in a highly cation-ordered double-perovskite insulator Sr3OsO6 journal, February 2019

Coexistence of metallic and nonmetallic properties in the pyrochlore Lu2Rh2O7 journal, March 2019

A suite-level review of the neutron powder diffraction instruments at Oak Ridge National Laboratory journal, September 2018

Topological properties and functionalities in oxide thin films and interfaces journal, March 2018

First-principles studies of spin-orbital physics in pyrochlore oxides journal, May 2019

Spin-orbit coupling induced magnetic anisotropy and large spin wave gap in NaOsO 3 journal, November 2018

Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective journal, April 2019

Ultrafast dynamics in the Lifshitz-type 5 d pyrochlore antiferromagnet Cd 2 Os 2 O 7 journal, October 2019

Coupled spin-charge-phonon fluctuation in the all-in/all-out antiferromagnet Cd 2 Os 2 O 7 journal, December 2019

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 journal, January 2020

Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates journal, June 2018

Origin of magnetic excitation gap in double perovskite Sr 2 FeOsO 6 journal, December 2018

Spin-Orbit Coupling Controlled J = 3 / 2 Electronic Ground State in 5 d 3 Oxides journal, May 2017

Topological Properties and Functionalities in Oxide Thin Films and Interfaces text, January 2018

Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates text, January 2018

Ferromagnetism above 1000 K in highly cation-ordered double-perovskite insulator Sr3OsO6 text, January 2018

Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective text, January 2018

First-principles studies of spin-orbital physics in pyrochlore oxides text, January 2018

Coexistence of metallic and nonmetallic properties in the pyrochlore Lu$_2$Rh$_2$O$_7$ text, January 2019

Strain Induced Slater Transition in Polar Metal LiOsO$_3$ text, January 2019

Title: Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd₂Os₂O₇

Mott physics and band topology in materials with strong spin–orbit interaction
journal, March 2010

Novel $J_{eff} = 1 / 2$ Mott State Induced by Relativistic Spin-Orbit Coupling in ${Sr}_{2} {IrO}_{4}$
journal, August 2008

Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4
journal, March 2009

Topological semimetal and Fermi-arc surface states in the electronic structure of pyrochlore iridates
journal, May 2011

Correlated Quantum Phenomena in the Strong Spin-Orbit Regime
journal, March 2014

Noncollinear Magnetism and Spin-Orbit Coupling in $5 d$ Pyrochlore Oxide ${Cd}_{2} {Os}_{2} O_{7}$
journal, June 2012

Tetrahedral Magnetic Order and the Metal-Insulator Transition in the Pyrochlore Lattice of ${Cd}_{2} {Os}_{2} O_{7}$
journal, June 2012

Continuous metal-insulator transition in the pyrochlore ${Cd}_{2} {Os}_{2} O_{7}$
journal, April 2001

Searching for the Slater transition in the pyrochlore ${Cd}_{2} {Os}_{2} O_{7}$ with infrared spectroscopy
journal, July 2002

Orbital magnetism in Cd $_{2}$ Os $_{2}$ O $_{7}$ studied by x-ray magnetic circular dichroism
journal, November 2011

Magnetic Effects and the Hartree-Fock Equation
journal, May 1951

Anisotropy-Tuned Magnetic Order in Pyrochlore Iridates
journal, June 2015

Determination of long-range all-in-all-out ordering of Ir $^{4 +}$ moments in a pyrochlore iridate Eu $_{2}$ Ir $_{2}$ O $_{7}$ by resonant x-ray diffraction
journal, March 2013

Magnetic Field-Induced Insulator-Semimetal Transition in a Pyrochlore ${Nd}_{2} {Ir}_{2} O_{7}$
journal, July 2015

Magnetic Excitation Spectra of ${Sr}_{2} {IrO}_{4}$ Probed by Resonant Inelastic X-Ray Scattering: Establishing Links to Cuprate Superconductors
journal, April 2012

Large Spin-Wave Energy Gap in the Bilayer Iridate ${Sr}_{3} {Ir}_{2} O_{7}$ : Evidence for Enhanced Dipolar Interactions Near the Mott Metal-Insulator Transition
journal, October 2012

${CaIrO}_{3}$ : A Spin-Orbit Mott Insulator Beyond the $j_{eff} = 1 / 2$ Ground State
journal, April 2014

Testing the Validity of the Strong Spin-Orbit-Coupling Limit for Octahedrally Coordinated Iridate Compounds in a Model System ${Sr}_{3} {CuIrO}_{6}$
journal, October 2012

Crystal-Field Splitting and Correlation Effect on the Electronic Structure of $A_{2} {IrO}_{3}$
journal, February 2013

Excitonic quasiparticles in a spin–orbit Mott insulator
journal, July 2014

Magnetic order and electronic structure of the $5 d^{3}$ double perovskite ${Sr}_{2} {ScOsO}_{6}$
journal, March 2015

Magnetic State of Pyrochlore ${Cd}_{2} {Os}_{2} O_{7}$ Emerging from Strong Competition of Ligand Distortions and Longer-Range Crystalline Anisotropy
journal, March 2013

Strong Correlations from Hund’s Coupling
journal, April 2013

Resonant inelastic x-ray scattering studies of elementary excitations
journal, June 2011

The high-resolution powder diffractometer at the high flux isotope reactor
journal, March 2010

A new protocol for the determination of magnetic structures using simulated annealing and representational analysis (SARAh)
journal, March 2000

Momentum-resolved Resonant and Nonresonant Inelastic X-ray Scattering at the Advanced Photon Source
journal, November 2009

Excitonic quasiparticles in a spin–orbit Mott insulator
journal, July 2014

Longer-range lattice anisotropy strongly competing with spin-orbit interactions in pyrochlore iridates
journal, March 2014

Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr2IrO4
journal, March 2009

[OsF ₆ ] ^{x −} : Molecular Models for Spin-Orbit Entangled Phenomena
journal, July 2017

Neutron Instruments for Research in Coordination Chemistry: Neutron Instruments for Research in Coordination Chemistry
journal, January 2019

Possible Origin of the Absence of Magnetic Order in LiOsO ₃ : Spin–Orbit Coupling Controlled Ground State
journal, September 2018

Strain‐Induced Slater Transition in Polar Metal LiOsO ₃
journal, May 2019

Ferromagnetism above 1000 K in a highly cation-ordered double-perovskite insulator Sr3OsO6
journal, February 2019

Coexistence of metallic and nonmetallic properties in the pyrochlore Lu2Rh2O7
journal, March 2019

A suite-level review of the neutron powder diffraction instruments at Oak Ridge National Laboratory
journal, September 2018

Topological properties and functionalities in oxide thin films and interfaces
journal, March 2018

First-principles studies of spin-orbital physics in pyrochlore oxides
journal, May 2019

Spin-orbit coupling induced magnetic anisotropy and large spin wave gap in NaOsO ₃
journal, November 2018

Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective
journal, April 2019

Ultrafast dynamics in the Lifshitz-type $5 d$ pyrochlore antiferromagnet ${Cd}_{2} {Os}_{2} O_{7}$
journal, October 2019

Coupled spin-charge-phonon fluctuation in the all-in/all-out antiferromagnet ${Cd}_{2} {Os}_{2} O_{7}$
journal, December 2019

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
journal, January 2020

Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates
journal, June 2018

Origin of magnetic excitation gap in double perovskite ${Sr}_{2} {FeOsO}_{6}$
journal, December 2018

Spin-Orbit Coupling Controlled $J = 3 / 2$ Electronic Ground State in $5 d^{3}$ Oxides
journal, May 2017

Topological Properties and Functionalities in Oxide Thin Films and Interfaces
text, January 2018

Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates
text, January 2018

Ferromagnetism above 1000 K in highly cation-ordered double-perovskite insulator Sr3OsO6
text, January 2018

Ultrafast dynamics of spin and orbital correlations in quantum materials: an energy- and momentum-resolved perspective
text, January 2018

First-principles studies of spin-orbital physics in pyrochlore oxides
text, January 2018

Coexistence of metallic and nonmetallic properties in the pyrochlore Lu$_2$Rh$_2$O$_7$
text, January 2019

Strain Induced Slater Transition in Polar Metal LiOsO$_3$
text, January 2019