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Title: Magnetism out of antisite disorder in the J = 0 compound Ba 2 YIrO 6

Abstract

Here, we systematically investigate the magnetic properties and local structure of Ba 2YIrO 6 to demonstrate that Y and Ir lattice defects in the form of antiphase boundary or clusters of antisite disorder affect the magnetism observed in this 5d 4 compound. The experimental investigation involved comparison of the magnetic properties and atomic imaging of (1) a slow-cooled crystal, (2) a crystal quenched from 900°C after growth, and (3) a crystal grown using a faster cooling rate during growth than the slow-cooled one. Atomic-scale imaging by scanning transmission electron microscopy (STEM) shows that quenching from 900°C introduces Ir-rich antiphase boundaries in the crystals, and a faster cooling rate during crystal growth leads to clusters of Y and Ir antisite disorder. Compared to the slow-cooled crystals, Ba 2YIrO 6 crystals with clusters of antisite defects have a larger effective moment and a larger saturation moment, while quenched crystals with Ir-rich antiphase boundary show a slightly suppressed moment. Our DFT and model magnetic Hamiltonian calculations suggest magnetic condensation is unlikely, as the energy to be gained from superexchange is small compared to the spin-orbit gap. However, once Y is replaced by Ir in the antisite disordered region, the picture of local nonmagneticmore » singlets breaks down and magnetism can be induced. This is because of (a) enhanced interactions due to increased orbital overlap and (b) increased number of orbitals mediating the interactions. Our work highlights the importance of lattice defects in understanding the experimentally observed magnetism in Ba 2YIrO 6 and other J = 0 systems.« less

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [3];  [4];  [1];  [5];  [2];  [2];  [2]; ORCiD logo [3]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. The Ohio State Univ., Columbus, OH (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  5. Univ. of Texas at Austin, Austin, TX (United States)
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) (SC-22)
OSTI Identifier:
1399964
Alternate Identifier(s):
OSTI ID: 1400010
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 96; Journal Issue: 14; 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

Citation Formats

Chen, Qiang, Svoboda, Chris, Zheng, Qiang, Sales, Brian C., Mandrus, David G., Zhou, H. D., Zhou, J. -S., McComb, David W., Randeria, Mohit, Trivedi, Nandini, and Yan, J. -Q. Magnetism out of antisite disorder in the J=0 compound Ba2YIrO6. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.96.144423.
Chen, Qiang, Svoboda, Chris, Zheng, Qiang, Sales, Brian C., Mandrus, David G., Zhou, H. D., Zhou, J. -S., McComb, David W., Randeria, Mohit, Trivedi, Nandini, & Yan, J. -Q. Magnetism out of antisite disorder in the J=0 compound Ba2YIrO6. United States. doi:10.1103/PhysRevB.96.144423.
Chen, Qiang, Svoboda, Chris, Zheng, Qiang, Sales, Brian C., Mandrus, David G., Zhou, H. D., Zhou, J. -S., McComb, David W., Randeria, Mohit, Trivedi, Nandini, and Yan, J. -Q. Wed . "Magnetism out of antisite disorder in the J=0 compound Ba2YIrO6". United States. doi:10.1103/PhysRevB.96.144423. https://www.osti.gov/servlets/purl/1399964.
@article{osti_1399964,
title = {Magnetism out of antisite disorder in the J=0 compound Ba2YIrO6},
author = {Chen, Qiang and Svoboda, Chris and Zheng, Qiang and Sales, Brian C. and Mandrus, David G. and Zhou, H. D. and Zhou, J. -S. and McComb, David W. and Randeria, Mohit and Trivedi, Nandini and Yan, J. -Q.},
abstractNote = {Here, we systematically investigate the magnetic properties and local structure of Ba2YIrO6 to demonstrate that Y and Ir lattice defects in the form of antiphase boundary or clusters of antisite disorder affect the magnetism observed in this 5d4 compound. The experimental investigation involved comparison of the magnetic properties and atomic imaging of (1) a slow-cooled crystal, (2) a crystal quenched from 900°C after growth, and (3) a crystal grown using a faster cooling rate during growth than the slow-cooled one. Atomic-scale imaging by scanning transmission electron microscopy (STEM) shows that quenching from 900°C introduces Ir-rich antiphase boundaries in the crystals, and a faster cooling rate during crystal growth leads to clusters of Y and Ir antisite disorder. Compared to the slow-cooled crystals, Ba2YIrO6 crystals with clusters of antisite defects have a larger effective moment and a larger saturation moment, while quenched crystals with Ir-rich antiphase boundary show a slightly suppressed moment. Our DFT and model magnetic Hamiltonian calculations suggest magnetic condensation is unlikely, as the energy to be gained from superexchange is small compared to the spin-orbit gap. However, once Y is replaced by Ir in the antisite disordered region, the picture of local nonmagnetic singlets breaks down and magnetism can be induced. This is because of (a) enhanced interactions due to increased orbital overlap and (b) increased number of orbitals mediating the interactions. Our work highlights the importance of lattice defects in understanding the experimentally observed magnetism in Ba2YIrO6 and other J = 0 systems.},
doi = {10.1103/PhysRevB.96.144423},
journal = {Physical Review B},
number = 14,
volume = 96,
place = {United States},
year = {2017},
month = {10}
}

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Works referenced in this record:

Electronic structure, local magnetism, and spin-orbit effects of Ir(IV)-, Ir(V)-, and Ir(VI)-based compounds
journal, June 2015


Magnetic and Transport Properties of the System La1-xSrxCoO3-δ (0 < x ≤ 0.50)
journal, September 1995

  • Senarı́s-Rodrıiguez, M.; Goodenough, J.
  • Journal of Solid State Chemistry, Vol. 118, Issue 2, p. 323-336
  • DOI: 10.1006/jssc.1995.1351

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

Cascade of Magnetic Field Induced Spin Transitions in LaCoO 3
journal, July 2012


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


An updated version of wannier90: A tool for obtaining maximally-localised Wannier functions
journal, August 2014

  • Mostofi, Arash A.; Yates, Jonathan R.; Pizzi, Giovanni
  • Computer Physics Communications, Vol. 185, Issue 8
  • DOI: 10.1016/j.cpc.2014.05.003

Diluted paramagnetic impurities in nonmagnetic Ba 2 YIrO 6
journal, October 2017


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


601. The magnetic properties of some d 4-complexes
journal, January 1961

  • Earnshaw, A.; Figgis, B. N.; Lewis, J.
  • Journal of the Chemical Society (Resumed)
  • DOI: 10.1039/jr9610003132

Observation of magnetic excitons in LaCoO 3
journal, June 2005


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


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


Low temperature Schottky anomalies in the specific heat of LaCoO3: Defect-stabilized finite spin states
journal, March 2009

  • He, C.; Zheng, H.; Mitchell, J. F.
  • Applied Physics Letters, Vol. 94, Issue 10
  • DOI: 10.1063/1.3098374

Evidence for a low-temperature magnetic ground state in double-perovskite iridates with I r 5 + ( 5 d 4 ) ions
journal, August 2017


Excitonic magnetism in d 6 perovskites
journal, March 2017


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


Bond-length fluctuations and the spin-state transition in L CoO 3 ( L = La , Pr, and Nd)
journal, April 2004


Insights into cationic ordering in Re-based double perovskite oxides
journal, January 2016

  • Lim, Tae-Won; Kim, Sung-Dae; Sung, Kil-Dong
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep19746

Cationic ordering control of magnetization in Sr2FeMoO6 double perovskite
journal, February 2001

  • Balcells, Ll.; Navarro, J.; Bibes, M.
  • Applied Physics Letters, Vol. 78, Issue 6
  • DOI: 10.1063/1.1346624

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


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


Electronic structure and spin-orbit driven magnetism in d 4.5 insulator Ba 3 YIr 2 O 9
journal, November 2015


Slater Insulator in Iridate Perovskites with Strong Spin-Orbit Coupling
journal, October 2016


Possible spin-orbit driven spin-liquid ground state in the double perovskite phase of Ba 3 YIr 2 O 9
journal, October 2013


An electron microscope for the aberration-corrected era
journal, February 2008


Ferromagnetism in La Co O 3
journal, July 2004


Ferromagnetic order in epitaxially strained La Co O 3 thin films
journal, April 2007


Quantitative STEM Imaging of Order-Disorder Phenomena in Double Perovskite Thin Films
journal, October 2016


Ferromagnetism in La Co O 3 nanoparticles
journal, November 2007


Spin state ordering of strongly correlating LaCoO 3 induced at ultrahigh magnetic fields
journal, June 2016


Fragile singlet ground-state magnetism in the pyrochlore osmates R 2 Os 2 O 7 ( R = Y and Ho)
journal, April 2016


Ferromagnetism at the surface of a La Co O 3 single crystal observed using scanning SQUID microscopy
journal, May 2007


Iridium double perovskite Sr 2 YIrO 6 : A combined structural and specific heat study
journal, February 2017


Strain-Induced Ferromagnetism and Magnetoresistance in Epitaxial Thin Films of LaCoO 3 Prepared by Polymer-Assisted Deposition
journal, December 2012

  • Rivadulla, Francisco; Bi, Zhenxing; Bauer, Eve
  • Chemistry of Materials, Vol. 25, Issue 1
  • DOI: 10.1021/cm3031472

    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

    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