DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Evidence for a low-temperature magnetic ground state in double-perovskite iridates with I r 5 + ( 5 d4 ) ions

Abstract

Here, we report an unusual magnetic ground state in single-crystal, double-perovskite Ba2YIrO6 and Sr-doped Ba2YIrO6 with Ir5+ (5d4) ions. Long-range magnetic order below 1.7 K is confirmed by dc magnetization, ac magnetic susceptibility, and heat-capacity measurements. The observed magnetic order is extraordinarily delicate and cannot be explained in terms of either a low-spin S=1 state, or a singlet Jeff=0 state imposed by the spin-orbit interactions (SOI). Alternatively, the magnetic ground state appears consistent with a SOI that competes with comparable Hund's rule coupling and inherently large electron hopping, which cannot stabilize the singlet Jeff=0 ground state. However, this picture is controversial, and conflicting magnetic behavior for these materials is reported in both experimental and theoretical studies, which highlights the intricate interplay of interactions that determine the ground state of materials with strong SOI.

Authors:
 [1];  [1]; ORCiD logo [2];  [1];  [3];  [4];  [4];  [1]
  1. Univ. of Colorado, Boulder, CO (United States). Dept. of Physics
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division; Univ. of Kentucky, Lexington, KY (United States). Dept. of Physics and Astronomy and Center for Advanced Materials
  3. Florida State Univ., Tallahassee, FL (United States). Dept. of Physics
  4. Univ. of Kentucky, Lexington, KY (United States). Dept. of Physics and Astronomy and Center for Advanced Materials
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1471893
Alternate Identifier(s):
OSTI ID: 1377642
Grant/Contract Number:  
AC05-00OR22725; FG02-98ER45707; DMR-1265162; DMR-1712101; DMR- 1506979
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 96; Journal Issue: 6; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE

Citation Formats

Terzic, Jasminka, Zheng, Hao, Ye, Feng, Zhao, H. D., Schlottmann, P., De Long, L. E., Yuan, S. J., and Cao, Gang. Evidence for a low-temperature magnetic ground state in double-perovskite iridates with Ir5+(5d4) ions. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.96.064436.
Terzic, Jasminka, Zheng, Hao, Ye, Feng, Zhao, H. D., Schlottmann, P., De Long, L. E., Yuan, S. J., & Cao, Gang. Evidence for a low-temperature magnetic ground state in double-perovskite iridates with Ir5+(5d4) ions. United States. https://doi.org/10.1103/PhysRevB.96.064436
Terzic, Jasminka, Zheng, Hao, Ye, Feng, Zhao, H. D., Schlottmann, P., De Long, L. E., Yuan, S. J., and Cao, Gang. Tue . "Evidence for a low-temperature magnetic ground state in double-perovskite iridates with Ir5+(5d4) ions". United States. https://doi.org/10.1103/PhysRevB.96.064436. https://www.osti.gov/servlets/purl/1471893.
@article{osti_1471893,
title = {Evidence for a low-temperature magnetic ground state in double-perovskite iridates with Ir5+(5d4) ions},
author = {Terzic, Jasminka and Zheng, Hao and Ye, Feng and Zhao, H. D. and Schlottmann, P. and De Long, L. E. and Yuan, S. J. and Cao, Gang},
abstractNote = {Here, we report an unusual magnetic ground state in single-crystal, double-perovskite Ba2YIrO6 and Sr-doped Ba2YIrO6 with Ir5+ (5d4) ions. Long-range magnetic order below 1.7 K is confirmed by dc magnetization, ac magnetic susceptibility, and heat-capacity measurements. The observed magnetic order is extraordinarily delicate and cannot be explained in terms of either a low-spin S=1 state, or a singlet Jeff=0 state imposed by the spin-orbit interactions (SOI). Alternatively, the magnetic ground state appears consistent with a SOI that competes with comparable Hund's rule coupling and inherently large electron hopping, which cannot stabilize the singlet Jeff=0 ground state. However, this picture is controversial, and conflicting magnetic behavior for these materials is reported in both experimental and theoretical studies, which highlights the intricate interplay of interactions that determine the ground state of materials with strong SOI.},
doi = {10.1103/PhysRevB.96.064436},
journal = {Physical Review B},
number = 6,
volume = 96,
place = {United States},
year = {Tue Aug 29 00:00:00 EDT 2017},
month = {Tue Aug 29 00:00:00 EDT 2017}
}

Journal Article:

Citation Metrics:
Cited by: 40 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Anomalous magnetic and transport behavior in the magnetic insulator Sr 3 Ir 2 O 7
journal, December 2002


Re-examination of the structure of Ba2MIrO6 (M=La, Y): space group revised
journal, May 2005


Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials
journal, March 2016


Determination of Hund's coupling in 5 d oxides using resonant inelastic x-ray scattering
journal, June 2017


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


Influence of structural distortions on the Ir magnetism in Ba2−xSrxYIrO6 double perovskites
journal, June 2016

  • Phelan, Brendan F.; Seibel, Elizabeth M.; Badoe, Daniel
  • Solid State Communications, Vol. 236
  • DOI: 10.1016/j.ssc.2016.03.017

A short history of SHELX
journal, December 2007

  • Sheldrick, George M.
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 64, Issue 1, p. 112-122
  • DOI: 10.1107/S0108767307043930

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


On the possibility of excitonic magnetism in Ir double perovskites
journal, January 2016


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


Spin–orbital locking, emergent pseudo-spin and magnetic order in honeycomb lattice iridates
journal, July 2012


Novel Magnetism of Ir 5 + ( 5 d 4 ) Ions in the Double Perovskite Sr 2 YIrO 6
journal, February 2014


Topological Quantum Phase Transition in 5 d Transition Metal Oxide Na 2 IrO 3
journal, March 2012


Novel magnetic state in d 4 Mott insulators
journal, February 2015


Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993


Engineering a Spin-Orbital Magnetic Insulator by Tailoring Superlattices
journal, June 2015


Weak ferromagnetism, metal-to-nonmetal transition, and negative differential resistivity in single-crystal Sr 2 IrO 4
journal, May 1998


Spin Waves and Revised Crystal Structure of Honeycomb Iridate Na 2 IrO 3
journal, March 2012


Structural and Magnetic Properties of the Iridium Double Perovskites Ba 2– x Sr x YIrO 6
journal, October 2015


Exotic phases induced by strong spin-orbit coupling in ordered double perovskites
journal, November 2010


Critical Properties of the Kitaev-Heisenberg Model
journal, November 2012


Excitonic Magnetism in Van Vleck–type d 4 Mott Insulators
journal, November 2013


Highly anisotropic exchange interactions of j eff = 1 2 iridium moments on the fcc lattice in La 2 B IrO 6   ( B = Mg , Zn )
journal, June 2016


J Freezing and Hund’s Rules in Spin-Orbit-Coupled Multiorbital Hubbard Models
journal, February 2017


NaIrO3—A pentavalent post-perovskite
journal, March 2011

  • Bremholm, M.; Dutton, S. E.; Stephens, P. W.
  • Journal of Solid State Chemistry, Vol. 184, Issue 3
  • DOI: 10.1016/j.jssc.2011.01.028

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


Ba 2 YIrO 6 : A cubic double perovskite material with Ir 5 + ions
journal, January 2016


Large- J approach to strongly coupled spin-orbital systems
journal, November 2009


Breakdown of J = 0 nonmagnetic state in d 4 iridate double perovskites: A first-principles study
journal, September 2015


Twisted Hubbard Model for Sr 2 IrO 4 : Magnetism and Possible High Temperature Superconductivity
journal, March 2011


Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides A 2 IrO 3
journal, July 2010


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


Über Sauerstoffperowskite mit fünf- und vierwertigem Iridium Verbindungen vom Typ Ba2B3+Ir5+O6 und Ba3B3+Ir4,5+2O9
journal, November 1980


Quantum Spin Hall Effect in a Transition Metal Oxide Na 2 IrO 3
journal, June 2009


Na 2 IrO 3 as a Molecular Orbital Crystal
journal, November 2012


Long-range magnetic ordering in Na 2 IrO 3
journal, June 2011


Spin-orbit coupled j eff = 1 / 2 iridium moments on the geometrically frustrated fcc lattice
journal, July 2015


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


Spin-orbit coupling in d 2 ordered double perovskites
journal, September 2011


Re-Examination of the Structure of Ba2MIrO6 (M: La, Y): Space Group Revised.
journal, August 2005


Large-J approach to strongly coupled spin-orbital systems
text, January 2009


Na2IrO3 as a molecular orbital crystal
text, January 2012


Critical properties of the Kitaev-Heisenberg model
text, January 2012


Correlated quantum phenomena in the strong spin-orbit regime
text, January 2013


Engineering spin-orbital magnetic insulator by tailoring superlattices
text, January 2014


Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials
text, January 2015


J-freezing and Hund's rules in spin-orbit-coupled multiorbital Hubbard models
text, January 2016


Works referencing / citing this record:

On J eff =0 Ground State Iridates(V): Tracking Residual Paramagnetism in New Bi 2 NaIrO 6
journal, October 2018

  • Prasad, Beluvalli E.; Doert, Thomas; Felser, Claudia
  • Chemistry - A European Journal, Vol. 24, Issue 63
  • DOI: 10.1002/chem.201804226

Orbiton–phonon coupling in Ir 5+ (5 d 4 ) double perovskite Ba 2 YIrO 6
journal, December 2018

  • Singh, Birender; Cansever, G. A.; Dey, T.
  • Journal of Physics: Condensed Matter, Vol. 31, Issue 6
  • DOI: 10.1088/1361-648x/aaf40a

The challenge of spin–orbit-tuned ground states in iridates: a key issues review
journal, February 2018


Nature of the magnetism of iridium in the double perovskite Sr 2 CoIrO 6
journal, July 2019


Ground state in the novel dimer iridate B a 13 I r 6 O 30 with I r 6 + ( 5 d 3 ) ions
journal, August 2019


Probing the J eff = 0 ground state and the Van Vleck paramagnetism of the Ir 5 + ions in layered Sr 2 Co 0.5 Ir 0.5 O 4
journal, June 2018


Block excitonic condensate at n = 3.5 in a spin-orbit coupled t 2 g multiorbital Hubbard model
journal, April 2019


Orbiton-Phonon coupling in Ir5+(5d4) double perovskite Ba2YIrO6
text, January 2017


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