skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Localized-itinerant dichotomy and unconventional magnetism in SrRu2O6

Abstract

Electron correlations tend to generate local magnetic moments that usually order if the lattices are not too frustrated. The hexagonal compound SrRu$$_2$$O$$_6$$ has a relatively high N{\'e}el temperature but small local moments, which seem to be at odds with the nominal valence of Ru$$^{5+}$$ in the $$t_{2g}^3$$ configuration. Here, we investigate the electronic and magnetic properties of SrRu$$_2$$O$$_6$$ using density functional theory (DFT) combined with dynamical mean field theory (DMFT). We find that the strong hybridization between Ru $d$ and O $p$ states results in a Ru valence that is closer to $+4$, leading to the small ordered moment, consistent with a DFT prediction. While the agreement with DFT might indicate that SrRu$$_2$$O$$_6$$ is in the weak coupling regime, our DMFT studies provide evidence from the mass enhancement and local moment formation that indicate correlation effects play a significant role. The local moment per Ru site is about a factor 2 larger than the ordered moment at low temperatures and remains finite in the whole temperature range investigated. Our theoretical N{\'e}el temperature $$\sim 700$$~K is in reasonable agreement with experimental observations. Due to a small lattice distortion, the degenerate $$t_{2g}$$ manifold is split and the quasiparticle weight is renormalized significantly in the $$a_{1g}$$ state, while correlation effects in $$e_g'$$ states are about a factor of 2--3 weaker. SrRu$$_2$$O$$_6$$ is a unique system in which localized and itinerant electrons coexist with the proximity to an orbitally-selective Mott transition within the $$t_{2g}$$ sector.

Authors:
; ; ; ;
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1394320
DOE Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Okamoto, Satoshi, Ochi, Masayuki, Arita, Ryotaro, Yan, Jiaqiang, and Trivedi, Nandini. Localized-itinerant dichotomy and unconventional magnetism in SrRu2O6. United States: N. p., 2017. Web. doi:10.1038/s41598-017-08503-y.
Okamoto, Satoshi, Ochi, Masayuki, Arita, Ryotaro, Yan, Jiaqiang, & Trivedi, Nandini. Localized-itinerant dichotomy and unconventional magnetism in SrRu2O6. United States. doi:10.1038/s41598-017-08503-y.
Okamoto, Satoshi, Ochi, Masayuki, Arita, Ryotaro, Yan, Jiaqiang, and Trivedi, Nandini. Wed . "Localized-itinerant dichotomy and unconventional magnetism in SrRu2O6". United States. doi:10.1038/s41598-017-08503-y.
@article{osti_1394320,
title = {Localized-itinerant dichotomy and unconventional magnetism in SrRu2O6},
author = {Okamoto, Satoshi and Ochi, Masayuki and Arita, Ryotaro and Yan, Jiaqiang and Trivedi, Nandini},
abstractNote = {Electron correlations tend to generate local magnetic moments that usually order if the lattices are not too frustrated. The hexagonal compound SrRu$_2$O$_6$ has a relatively high N{\'e}el temperature but small local moments, which seem to be at odds with the nominal valence of Ru$^{5+}$ in the $t_{2g}^3$ configuration. Here, we investigate the electronic and magnetic properties of SrRu$_2$O$_6$ using density functional theory (DFT) combined with dynamical mean field theory (DMFT). We find that the strong hybridization between Ru $d$ and O $p$ states results in a Ru valence that is closer to $+4$, leading to the small ordered moment, consistent with a DFT prediction. While the agreement with DFT might indicate that SrRu$_2$O$_6$ is in the weak coupling regime, our DMFT studies provide evidence from the mass enhancement and local moment formation that indicate correlation effects play a significant role. The local moment per Ru site is about a factor 2 larger than the ordered moment at low temperatures and remains finite in the whole temperature range investigated. Our theoretical N{\'e}el temperature $\sim 700$~K is in reasonable agreement with experimental observations. Due to a small lattice distortion, the degenerate $t_{2g}$ manifold is split and the quasiparticle weight is renormalized significantly in the $a_{1g}$ state, while correlation effects in $e_g'$ states are about a factor of 2--3 weaker. SrRu$_2$O$_6$ is a unique system in which localized and itinerant electrons coexist with the proximity to an orbitally-selective Mott transition within the $t_{2g}$ sector.},
doi = {10.1038/s41598-017-08503-y},
journal = {Scientific Reports},
issn = {2045-2322},
number = 1,
volume = 7,
place = {United States},
year = {2017},
month = {9}
}

Works referenced in this record:

Covalency in transition-metal oxides within all-electron dynamical mean-field theory
journal, August 2014


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


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


Ab initio calculations of quasiparticle band structure in correlated systems: LDA++ approach
journal, March 1998


Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
journal, November 2004


wannier90: A tool for obtaining maximally-localised Wannier functions
journal, May 2008

  • Mostofi, Arash A.; Yates, Jonathan R.; Lee, Young-Su
  • Computer Physics Communications, Vol. 178, Issue 9
  • DOI: 10.1016/j.cpc.2007.11.016

Nature of magnetic excitations in superconducting BaFe1.9Ni0.1As2
journal, March 2012

  • Liu, Mengshu; Harriger, Leland W.; Luo, Huiqian
  • Nature Physics, Vol. 8, Issue 5
  • DOI: 10.1038/nphys2268

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


Bayesian inference and the analytic continuation of imaginary-time quantum Monte Carlo data
journal, May 1996


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

  • Hiley, Craig I.; Lees, Martin R.; Fisher, Janet M.
  • Angewandte Chemie International Edition, Vol. 53, Issue 17
  • DOI: 10.1002/anie.201310110

Antiferromagnetism. Theory of Superexchange Interaction
journal, July 1950


Maximally localized generalized Wannier functions for composite energy bands
journal, November 1997


Dichotomy between Large Local and Small Ordered Magnetic Moments in Iron-Based Superconductors
journal, May 2010


Spin-orbit-induced orbital excitations in Sr 2 RuO 4 and Ca 2 RuO 4 : A resonant inelastic x-ray scattering study
journal, April 2015


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


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
  • DOI: 10.1088/0953-8984/9/4/002

Janus-Faced Influence of Hund’s Rule Coupling in Strongly Correlated Materials
journal, December 2011


Continuous metal-insulator transition of the antiferromagnetic perovskite NaOsO 3
journal, October 2009


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


First-principles calculations of the electronic structure and spectra of strongly correlated systems: dynamical mean-field theory
journal, September 1997

  • Anisimov, V. I.; Poteryaev, A. I.; Korotin, M. A.
  • Journal of Physics: Condensed Matter, Vol. 9, Issue 35
  • DOI: 10.1088/0953-8984/9/35/010

Magnetic Structure of the Cubic Perovskite Type SrMnO 3
journal, July 1974

  • Takeda, Takayoshi; Ōhara, Sōji
  • Journal of the Physical Society of Japan, Vol. 37, Issue 1
  • DOI: 10.1143/JPSJ.37.275

Electronic structure calculations with dynamical mean-field theory
journal, August 2006


Dynamical mean-field theory within the full-potential methods: Electronic structure of CeIrIn 5 , CeCoIn 5 , and CeRhIn 5
journal, May 2010


Finite-Temperature Magnetism of Transition Metals: An ab initio Dynamical Mean-Field Theory
journal, July 2001


Origin of the High Néel Temperature in SrTcO 3
journal, May 2012


The Basis of the Electron Theory of Metals, with Special Reference to the Transition Metals
journal, July 1949


Continuous-Time Solver for Quantum Impurity Models
journal, August 2006


High Temperature Magnetic Ordering in the 4 d Perovskite SrTcO 3
journal, February 2011


Exact Double Counting in Combining the Dynamical Mean Field Theory and the Density Functional Theory
journal, November 2015


High-Spin to Low-Spin and Orbital Polarization Transitions in Multiorbital Mott Systems
journal, September 2007


High antiferromagnetic transition temperature of the honeycomb compound SrRu 2 O 6
journal, September 2015


Effective magnetic interactions in spin-orbit coupled d 4 Mott insulators
journal, January 2017


Spin State of Negative Charge-Transfer Material SrCoO 3
journal, September 2012


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


The crystal and magnetic structures of Sr2YRuO6
journal, April 1984


Theory of High T c Ferrimagnetism in a Multiorbital Mott Insulator
journal, February 2013


Local-density functional and on-site correlations: The electronic structure of La 2 CuO 4 and LaCuO 3
journal, May 1994


Wien2wannier: From linearized augmented plane waves to maximally localized Wannier functions
journal, November 2010

  • Kuneš, Jan; Arita, Ryotaro; Wissgott, Philipp
  • Computer Physics Communications, Vol. 181, Issue 11
  • DOI: 10.1016/j.cpc.2010.08.005

The crystal structures and magnetic properties of Ba2LaRuO6 and Ca2LaRuO6
journal, February 1983


Hybridization expansion impurity solver: General formulation and application to Kondo lattice and two-orbital models
journal, October 2006


Quantum dynamical screening of the local magnetic moment in Fe-based superconductors
journal, August 2012


Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992


Orbital-Selective Mott Transition out of Band Degeneracy Lifting
journal, March 2009


Dynamical mean-field theory of strongly correlated fermion systems and the limit of infinite dimensions
journal, January 1996

  • Georges, Antoine; Kotliar, Gabriel; Krauth, Werner
  • Reviews of Modern Physics, Vol. 68, Issue 1
  • DOI: 10.1103/RevModPhys.68.13

Strong Correlations from Hund’s Coupling
journal, April 2013


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


Semiconductor-metal transition in novel Cd2Os2O7
journal, February 1974


Maximally localized Wannier functions for entangled energy bands
journal, December 2001