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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:
 [1];  [2];  [3];  [4];  [5];  [6];  [6];  [7];  [6];  [8];  [8];  [8];  [9];  [9];  [10];  [5];  [11]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
  2. Univ. College London (UCL), London (United Kingdom). London Centre for Nanotechnology
  3. Leibniz Inst. for Solid State and Materials Research (IFW), Dresden (Germany)
  4. 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)
  5. Univ. College London (UCL), London (United Kingdom). London Centre for Nanotechnology
  6. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  7. Argonne National Laboratory (ANL), Advanced Photon Source (APS)
  8. 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
  9. Leibniz Inst. for Solid State and Materials Research (IFW), Dresden (Germany); Technische Univ. Dresden (Germany)
  10. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
  11. 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:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); 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.
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. doi:10.1038/ncomms11651.
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. doi:10.1038/ncomms11651. https://www.osti.gov/servlets/purl/1338574.
@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 = {2016},
month = {6}
}

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Works referenced in this record:

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    Works referencing / citing this record:

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

    • Pedersen, Kasper S.; Woodruff, Daniel N.; Singh, Saurabh Kumar
    • Chemistry - A European Journal, Vol. 23, Issue 47
    • DOI: 10.1002/chem.201702894

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

    • Cao, Y.; Mazzone, D. G.; Meyers, D.
    • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145
    • DOI: 10.1098/rsta.2017.0480

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

    • Pedersen, Kasper S.; Woodruff, Daniel N.; Singh, Saurabh Kumar
    • Chemistry - A European Journal, Vol. 23, Issue 47
    • DOI: 10.1002/chem.201702894

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

    • Cao, Y.; Mazzone, D. G.; Meyers, D.
    • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145
    • DOI: 10.1098/rsta.2017.0480