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Title: Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet

Abstract

Ruthenium compounds serve as a platform for fundamental concepts such as spin-triplet superconductivity, Kitaev spin liquids and solid-state analogues of the Higgs mode in particle physics. However, basic questions about the electronic structure of ruthenates remain unanswered, because several key parameters (including Hund’s coupling, spin–orbit coupling and exchange interactions) are comparable in magnitude and their interplay is poorly understood, partly due to difficulties in synthesizing large single crystals for spectroscopic experiments. Here we introduce a resonant inelastic X-ray scattering (RIXS) technique capable of probing collective modes in microcrystals of 4d electron materials. We observe spin waves and spin-state transitions in the honeycomb antiferromagnet SrRu2O6 (ref. 10) and use the extracted exchange interactions and measured magnon gap to explain its high Néel temperature. We expect that the RIXS method presented here will enable momentum-resolved spectroscopy of a large class of 4d transition-metal compounds.

Authors:
ORCiD logo [1];  [2];  [3];  [1];  [1];  [1];  [4];  [1]; ORCiD logo [1];  [1];  [5];  [5];  [5]; ORCiD logo [1]; ORCiD logo [6];  [4]; ORCiD logo [1]; ORCiD logo [7]; ORCiD logo [1]
  1. Max-Planck-Inst. fur Festkorperforschung, Stuttgart (Germany)
  2. Max-Planck-Inst. fur Festkorperforschung, Stuttgart (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  3. Max-Planck-Inst. fur Festkorperforschung, Stuttgart (Germany); Univ. Stuttgart, Stuttgart (Germany)
  4. Max-Planck-Inst. fur Festkorperforschung, Stuttgart (Germany); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of); Center for Artificial Low Dimensional Electronic Systems, Inst. for Basic Science (IBS), Pohang (South Korea)
  5. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  6. Max-Planck-Inst. fur Festkorperforschung, Stuttgart (Germany); Univ. Stuttgart, Stuttgart (Germany); Univ. of Tokyo (Japan)
  7. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1532472
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 18; Journal Issue: 6; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Suzuki, H., Gretarsson, H., Ishikawa, H., Ueda, K., Yang, Z., Liu, H., Kim, H., Kukusta, D., Yaresko, A., Minola, M., Sears, J. A., Francoual, S., Wille, H. -C., Nuss, J., Takagi, H., Kim, B. J., Khaliullin, G., Yavaş, H., and Keimer, B. Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet. United States: N. p., 2019. Web. doi:10.1038/s41563-019-0327-2.
Suzuki, H., Gretarsson, H., Ishikawa, H., Ueda, K., Yang, Z., Liu, H., Kim, H., Kukusta, D., Yaresko, A., Minola, M., Sears, J. A., Francoual, S., Wille, H. -C., Nuss, J., Takagi, H., Kim, B. J., Khaliullin, G., Yavaş, H., & Keimer, B. Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet. United States. https://doi.org/10.1038/s41563-019-0327-2
Suzuki, H., Gretarsson, H., Ishikawa, H., Ueda, K., Yang, Z., Liu, H., Kim, H., Kukusta, D., Yaresko, A., Minola, M., Sears, J. A., Francoual, S., Wille, H. -C., Nuss, J., Takagi, H., Kim, B. J., Khaliullin, G., Yavaş, H., and Keimer, B. Mon . "Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet". United States. https://doi.org/10.1038/s41563-019-0327-2. https://www.osti.gov/servlets/purl/1532472.
@article{osti_1532472,
title = {Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet},
author = {Suzuki, H. and Gretarsson, H. and Ishikawa, H. and Ueda, K. and Yang, Z. and Liu, H. and Kim, H. and Kukusta, D. and Yaresko, A. and Minola, M. and Sears, J. A. and Francoual, S. and Wille, H. -C. and Nuss, J. and Takagi, H. and Kim, B. J. and Khaliullin, G. and Yavaş, H. and Keimer, B.},
abstractNote = {Ruthenium compounds serve as a platform for fundamental concepts such as spin-triplet superconductivity, Kitaev spin liquids and solid-state analogues of the Higgs mode in particle physics. However, basic questions about the electronic structure of ruthenates remain unanswered, because several key parameters (including Hund’s coupling, spin–orbit coupling and exchange interactions) are comparable in magnitude and their interplay is poorly understood, partly due to difficulties in synthesizing large single crystals for spectroscopic experiments. Here we introduce a resonant inelastic X-ray scattering (RIXS) technique capable of probing collective modes in microcrystals of 4d electron materials. We observe spin waves and spin-state transitions in the honeycomb antiferromagnet SrRu2O6 (ref. 10) and use the extracted exchange interactions and measured magnon gap to explain its high Néel temperature. We expect that the RIXS method presented here will enable momentum-resolved spectroscopy of a large class of 4d transition-metal compounds.},
doi = {10.1038/s41563-019-0327-2},
journal = {Nature Materials},
number = 6,
volume = 18,
place = {United States},
year = {Mon Mar 25 00:00:00 EDT 2019},
month = {Mon Mar 25 00:00:00 EDT 2019}
}

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Works referenced in this record:

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journal, January 2012

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Raman Scattering from Higgs Mode Oscillations in the Two-Dimensional Antiferromagnet Ca 2 RuO 4
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Resonant inelastic x-ray scattering spectra for electrons in solids
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High antiferromagnetic transition temperature of the honeycomb compound SrRu 2 O 6
journal, September 2015


Antiferromagnetism at T > 500 K in the layered hexagonal ruthenate SrR u 2 O 6
journal, September 2015


Localized itinerant electrons and unique magnetic properties of SrRu 2 O 6
journal, October 2015


Electronic structure and the origin of the high ordering temperature in SrRu 2 O 6
journal, June 2015


DFT+DMFT study on soft moment magnetism and covalent bonding in SrRu 2 O 6
journal, October 2017


Localized-itinerant dichotomy and unconventional magnetism in SrRu2O6
journal, September 2017


Dispersion of Magnetic Excitations in the Cuprate La 2 CuO 4 and CaCuO 2 Compounds Measured Using Resonant X-Ray Scattering
journal, April 2009


Resonant inelastic x-ray scattering operators for t 2 g orbital systems
journal, August 2017


Ruthenium(V) Oxides from Low-Temperature Hydrothermal Synthesis
journal, March 2014

  • Hiley, Craig I.; Lees, Martin R.; Fisher, Janet M.
  • Angewandte Chemie, Vol. 126, Issue 17
  • DOI: 10.1002/ange.201310110

Localized itinerant electrons and unique magnetic properties of SrRu2O6
text, January 2015


Resonant inelastic x-ray scattering operators for $t_{2g}$ orbital systems
text, January 2017


Higgs mode and its decay in a two dimensional antiferromagnet
text, January 2017


DFT+DMFT study on soft moment magnetism and covalent bonding in SrRu$_2$O$_6$
text, January 2017


Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009


Works referencing / citing this record:

Resonant inelastic x-ray scattering study of $\alpha$ -RuCl 3 : a progress report
journal, January 2020

  • Lebert, Blair W.; Kim, Subin; Bisogni, Valentina
  • Journal of Physics: Condensed Matter, Vol. 32, Issue 14
  • DOI: 10.1088/1361-648x/ab5595

Observation of spin-orbit excitations and Hund's multiplets in Ca 2 RuO 4
journal, July 2019


Raman scattering from current-stabilized nonequilibrium phases in Ca 2 RuO 4
journal, August 2019


Proximate ferromagnetic state in the Kitaev model material $\alpha$-RuCl$_3$
text, January 2021


Spin and charge excitations in the correlated multiband metal Ca3Ru2O7
text, January 2020


Magnetic and electronic ordering phenomena in the [Ru$_2$O$_6$] honeycomb lattice compound AgRuO$_3$
text, January 2021