The Crystal Structure and Magnetic Behavior of Quinary Osmate and Ruthenate Double Perovskites La ABB'O 6 (A = Ca, Sr; B = Co, Ni; B' = Ru, Os)

Morrow, Ryan; McGuire, Michael A.; Yan, Jiaqiang; Woodward, Patrick M.

doi:10.1021/acs.inorgchem.7b02282

Title: The Crystal Structure and Magnetic Behavior of Quinary Osmate and Ruthenate Double Perovskites La ABB'O ₆ (A = Ca, Sr; B = Co, Ni; B' = Ru, Os)

Abstract

In this work, six LaABB'O₆ (A = Ca, Sr; B = Co, Ni; B' = Ru, Os) double perovskites were synthesized, several for the first time, and their crystal structures and magnetic behavior were characterized with neutron powder diffraction and direct-current and alternating-current magnetometry. All six compounds crystallize with P2₁/n space group symmetry, resulting from a^–a^–c⁺ octahedral tilting and complete rock salt ordering of transition-metal ions. Despite the electronic configurations of the transition-metal ions, either d⁸–d³ or d⁷–d³, not one of the six compounds shows ferromagnetism as predicted by the Goodenough–Kanamori rules. LaSrNiOsO₆, LaSrNiRuO₆, and LaCaNiRuO₆ display long-range antiferromagnetic order, while LaCaNiOsO₆, LaCaCoOsO₆, and LaSrCoOsO₆ exhibit spin-glass behavior. These compounds are compared to the previously studied LaCaCoRuO₆ and LaSrCoRuO₆, both of which order antiferromagnetically. Lastly, the observed variations in magnetic properties can be attributed largely to the response of competing superexchange pathways due to changes in B–O–B' bond angles, differences in the radial extent of the 4d (B' = Ru) and 5d (B' = Os) orbitals, and filling of the t_2g orbitals of the 3d ion.

Authors:

^[1];

^[2];

^[3];

^[1]

The Ohio State Univ., Columbus, OH (United States). Department of Chemistry and Biochemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division; Univ. of Tennessee, Knoxville, TN (United States). Department of Materials Science and Engineering

Publication Date:: 2018-02-23

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

OSTI Identifier:: 1427710

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Inorganic Chemistry

Additional Journal Information:: Journal Volume: 57; Journal Issue: 6; Journal ID: ISSN 0020-1669

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Morrow, Ryan, McGuire, Michael A., Yan, Jiaqiang, and Woodward, Patrick M.. The Crystal Structure and Magnetic Behavior of Quinary Osmate and Ruthenate Double Perovskites La ABB'O 6 (A = Ca, Sr; B = Co, Ni; B' = Ru, Os).  United States: N. p., 2018. 
Web.  doi:10.1021/acs.inorgchem.7b02282.

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                    Morrow, Ryan, McGuire, Michael A., Yan, Jiaqiang, & Woodward, Patrick M.. The Crystal Structure and Magnetic Behavior of Quinary Osmate and Ruthenate Double Perovskites La ABB'O 6 (A = Ca, Sr; B = Co, Ni; B' = Ru, Os).  United States.  https://doi.org/10.1021/acs.inorgchem.7b02282

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                    Morrow, Ryan, McGuire, Michael A., Yan, Jiaqiang, and Woodward, Patrick M.. Fri .  
"The Crystal Structure and Magnetic Behavior of Quinary Osmate and Ruthenate Double Perovskites La ABB'O 6 (A = Ca, Sr; B = Co, Ni; B' = Ru, Os)".  United States.  https://doi.org/10.1021/acs.inorgchem.7b02282.  https://www.osti.gov/servlets/purl/1427710.

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@article{osti_1427710,

  title        = {The Crystal Structure and Magnetic Behavior of Quinary Osmate and Ruthenate Double Perovskites La ABB'O 6 (A = Ca, Sr; B = Co, Ni; B' = Ru, Os)},

  author       = {Morrow, Ryan and McGuire, Michael A. and Yan, Jiaqiang and Woodward, Patrick M.},

  abstractNote = {In this work, six LaABB'O6 (A = Ca, Sr; B = Co, Ni; B' = Ru, Os) double perovskites were synthesized, several for the first time, and their crystal structures and magnetic behavior were characterized with neutron powder diffraction and direct-current and alternating-current magnetometry. All six compounds crystallize with P21/n space group symmetry, resulting from a–a–c+ octahedral tilting and complete rock salt ordering of transition-metal ions. Despite the electronic configurations of the transition-metal ions, either d8–d3 or d7–d3, not one of the six compounds shows ferromagnetism as predicted by the Goodenough–Kanamori rules. LaSrNiOsO6, LaSrNiRuO6, and LaCaNiRuO6 display long-range antiferromagnetic order, while LaCaNiOsO6, LaCaCoOsO6, and LaSrCoOsO6 exhibit spin-glass behavior. These compounds are compared to the previously studied LaCaCoRuO6 and LaSrCoRuO6, both of which order antiferromagnetically. Lastly, the observed variations in magnetic properties can be attributed largely to the response of competing superexchange pathways due to changes in B–O–B' bond angles, differences in the radial extent of the 4d (B' = Ru) and 5d (B' = Os) orbitals, and filling of the t2g orbitals of the 3d ion.},

  doi          = {10.1021/acs.inorgchem.7b02282},

  journal      = {Inorganic Chemistry},

  number       = 6,

  volume       = 57,

  place        = {United States},

  year         = {2018},

  month        = {2}

}

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https://doi.org/10.1021/acs.inorgchem.7b02282

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Figure 1: The upper half depicts AFM-I and AFM-II structures commonly found on the double perovskite pseudo FCC when only either B or B’ is a magnetic transition metal cation. For AFM-I, any given magnetic cation has 8 NN AFM pairs and 4 FM NN pairs while having 6 FMmore »

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Title: The Crystal Structure and Magnetic Behavior of Quinary Osmate and Ruthenate Double Perovskites La ABB'O 6 (A = Ca, Sr; B = Co, Ni; B' = Ru, Os)

Abstract

Citation Formats

Figures / Tables:

Cation ordering in perovskites journal, January 2010

A2B′B″O6 perovskites: A review journal, May 2015

Room-temperature magnetoresistance in an oxide material with an ordered double-perovskite structure journal, October 1998

Multiferroic thin film of Bi2NiMnO6 with ordered double-perovskite structure journal, February 2007

Erratum: Sr 2 Cr Os O 6 : End point of a spin-polarized metal-insulator transition by 5 d band filling [Phys. Rev. B 75 , 020404(R) (2007)] journal, May 2007

The effect of chemical pressure on the structure and properties of A2CrOsO6 (A=Sr, Ca) ferrimagnetic double perovskite journal, June 2016

Metallic ordered double-perovskite Sr2CrReO6 with maximal Curie temperature of 635 K journal, July 2002

Theory of the Role of Covalence in the Perovskite-Type Manganites [ La , M ( II ) ] Mn O 3 journal, October 1955

Superexchange interaction and symmetry properties of electron orbitals journal, July 1959

Magnetic structures of fcc systems with nearest-neighbor and next-nearest-neighbor exchange interactions journal, December 1988

Matrix elements of four-quark operators relevant to life time difference $\Delta \Gamma _{B_s}$ from QCD sum rules journal, June 2001

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

Spin-orbit coupling controlled ground state in Sr 2 ScOsO 6 journal, June 2016

Spin-orbit coupling control of anisotropy, ground state and frustration in 5d2 Sr2MgOsO6 journal, August 2016

Magnetic order and electronic structure of the 5 d 3 double perovskite Sr 2 ScOsO 6 journal, March 2015

Structure and Magnetic Properties of Sr 2 CoWO 6 : An Ordered Double Perovskite Containing Co 2+ (HS) with Unquenched Orbital Magnetic Moment journal, April 2003

Synthesis, Crystal and Magnetic Structure of the Double Perovskites A2NiMoO6 (A = Sr, Ba): A Neutron Diffraction Study journal, August 2003

Oxygen stoichiometry, ferromagnetism, and transport properties of La 2 − x NiMnO 6 + δ journal, August 2003

Magnetocapacitance and Magnetoresistance Near Room Temperature in a Ferromagnetic Semiconductor: La2NiMnO6 journal, September 2005

Designed Ferromagnetic, Ferroelectric Bi 2 NiMnO 6 journal, June 2005

Composition-controlled metal-insulator transitions and minimum metallic conductivity in the oxide systems LaNi1−xMxO3 (M = Cr, Mn, Fe, or Co) journal, October 1984

Magnetism in Ca 2 CoOsO 6 and Ca 2 NiOsO 6 : Unraveling the Mystery of Superexchange Interactions between 3d and 5d Ions journal, May 2016

Lattice Instability and Competing Spin Structures in the Double Perovskite Insulator Sr 2 FeOsO 6 journal, October 2013

Independent Ordering of Two Interpenetrating Magnetic Sublattices in the Double Perovskite Sr 2 CoOsO 6 journal, December 2013

Lattice-Site-Specific Spin Dynamics in Double Perovskite Sr 2 CoOsO 6 journal, April 2014

Probing the Links between Structure and Magnetism in Sr 2– x Ca x FeOsO 6 Double Perovskites journal, July 2014

High-Temperature Ferrimagnetism Driven by Lattice Distortion in Double Perovskite Ca 2 FeOsO 6 journal, February 2014

Effects of chemical pressure on the magnetic ground states of the osmate double perovskites SrCaCoOs O 6 and C a 2 CoOs O 6 journal, September 2015

Structural, Magnetic, and Transport Properties of (La 1+ x Sr 1- x )CoRuO 6 Double Perovskites journal, May 2004

Control of antisite disorder, magnetism, and asymmetric doping effects in (La1+xCa1-x)CoRuO6 double perovskites journal, March 2004

EXPGUI , a graphical user interface for GSAS journal, April 2001

A new protocol for the determination of magnetic structures using simulated annealing and representational analysis (SARAh) journal, March 2000

Structure determination of A 2 M 3+ TaO 6 and A 2 M 3+ NbO 6 ordered perovskites: octahedral tilting and pseudosymmetry journal, May 2006

Structure prediction of ordered and disordered multiple octahedral cation perovskites using SPuDS journal, May 2006

The classification of tilted octahedra in perovskites journal, November 1972

Bond-valence parameters for solids journal, April 1991

Synthesis, Structure, and Magnetic Properties of Sr2NiOsO6 and Ca2NiOsO6: Two New Osmium-Containing Double Perovskites journal, November 2005

Magnetic properties of the S = 3 2 geometrically frustrated double perovskites La 2 LiRuO 6 and Ba 2 YRuO 6 journal, October 2009

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal, September 1976

Die Gesetze der Krystallochemie journal, May 1926

Synthesis, Crystal Structure, and Properties of the Ordered Double Perovskite Sr 2 CoOsO 6 : Ordered Double Perovskite Sr journal, September 2013

Synthesis, crystal structures, and magnetic properties of double perovskites SrLaNiOsO6 and BaLaNiOsO6 journal, October 2016

B a 2 NiOs O 6 : A Dirac-Mott insulator with ferromagnetism near 100 K journal, December 2016

Synthesis, structure, and magnetic properties of novel B-site ordered double perovskites, SrLaMReO 6 (M = Mg, Mn, Co and Ni) journal, January 2015

‘A’ cation control of perovskite properties journal, September 2002

Title: The Crystal Structure and Magnetic Behavior of Quinary Osmate and Ruthenate Double Perovskites La ABB'O ₆ (A = Ca, Sr; B = Co, Ni; B' = Ru, Os)

Cation ordering in perovskites
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A2B′B″O6 perovskites: A review
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Room-temperature magnetoresistance in an oxide material with an ordered double-perovskite structure
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Multiferroic thin film of Bi2NiMnO6 with ordered double-perovskite structure
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Erratum: ${Sr}_{2} Cr Os O_{6}$ : End point of a spin-polarized metal-insulator transition by $5 d$ band filling [Phys. Rev. B 75 , 020404(R) (2007)]
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The effect of chemical pressure on the structure and properties of A2CrOsO6 (A=Sr, Ca) ferrimagnetic double perovskite
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Metallic ordered double-perovskite Sr2CrReO6 with maximal Curie temperature of 635 K
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Theory of the Role of Covalence in the Perovskite-Type Manganites $[La, M (II)] Mn O_{3}$
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Superexchange interaction and symmetry properties of electron orbitals
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Magnetic structures of fcc systems with nearest-neighbor and next-nearest-neighbor exchange interactions
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Matrix elements of four-quark operators relevant to life time difference $\Delta \Gamma _{B_s}$ from QCD sum rules
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The crystal structures and magnetic properties of Ba2LaRuO6 and Ca2LaRuO6
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Spin-orbit coupling controlled ground state in ${Sr}_{2} {ScOsO}_{6}$
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Spin-orbit coupling control of anisotropy, ground state and frustration in 5d2 Sr2MgOsO6
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Magnetic order and electronic structure of the $5 d^{3}$ double perovskite ${Sr}_{2} {ScOsO}_{6}$
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Structure and Magnetic Properties of Sr ₂ CoWO ₆ : An Ordered Double Perovskite Containing Co ²⁺ (HS) with Unquenched Orbital Magnetic Moment
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Synthesis, Crystal and Magnetic Structure of the Double Perovskites A2NiMoO6 (A = Sr, Ba): A Neutron Diffraction Study
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Oxygen stoichiometry, ferromagnetism, and transport properties of ${La}_{2 - x} {NiMnO}_{6 + δ}$
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Magnetocapacitance and Magnetoresistance Near Room Temperature in a Ferromagnetic Semiconductor: La2NiMnO6
journal, September 2005

Designed Ferromagnetic, Ferroelectric Bi ₂ NiMnO ₆
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Composition-controlled metal-insulator transitions and minimum metallic conductivity in the oxide systems LaNi1−xMxO3 (M = Cr, Mn, Fe, or Co)
journal, October 1984

Magnetism in Ca ₂ CoOsO ₆ and Ca ₂ NiOsO ₆ : Unraveling the Mystery of Superexchange Interactions between 3d and 5d Ions
journal, May 2016

Lattice Instability and Competing Spin Structures in the Double Perovskite Insulator ${Sr}_{2} {FeOsO}_{6}$
journal, October 2013

Independent Ordering of Two Interpenetrating Magnetic Sublattices in the Double Perovskite Sr ₂ CoOsO ₆
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Lattice-Site-Specific Spin Dynamics in Double Perovskite ${Sr}_{2} {CoOsO}_{6}$
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Probing the Links between Structure and Magnetism in Sr _{2– x} Ca _x FeOsO ₆ Double Perovskites
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High-Temperature Ferrimagnetism Driven by Lattice Distortion in Double Perovskite Ca ₂ FeOsO ₆
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Effects of chemical pressure on the magnetic ground states of the osmate double perovskites $SrCaCoOs O_{6}$ and $C a_{2} CoOs O_{6}$
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Structural, Magnetic, and Transport Properties of (La ₁₊ _x Sr _1- _x )CoRuO ₆ Double Perovskites
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Control of antisite disorder, magnetism, and asymmetric doping effects in (La1+xCa1-x)CoRuO6 double perovskites
journal, March 2004

EXPGUI , a graphical user interface for GSAS
journal, April 2001

A new protocol for the determination of magnetic structures using simulated annealing and representational analysis (SARAh)
journal, March 2000

Structure determination of A ₂ M ³⁺ TaO ₆ and A ₂ M ³⁺ NbO ₆ ordered perovskites: octahedral tilting and pseudosymmetry
journal, May 2006

Structure prediction of ordered and disordered multiple octahedral cation perovskites using SPuDS
journal, May 2006

The classification of tilted octahedra in perovskites
journal, November 1972

Bond-valence parameters for solids
journal, April 1991

Synthesis, Structure, and Magnetic Properties of Sr₂NiOsO₆ and Ca₂NiOsO₆: Two New Osmium-Containing Double Perovskites
journal, November 2005

Magnetic properties of the $S = \frac{3}{2}$ geometrically frustrated double perovskites ${La}_{2} {LiRuO}_{6}$ and ${Ba}_{2} {YRuO}_{6}$
journal, October 2009

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

Die Gesetze der Krystallochemie
journal, May 1926

Synthesis, Crystal Structure, and Properties of the Ordered Double Perovskite Sr ₂ CoOsO ₆ : Ordered Double Perovskite Sr
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Synthesis, crystal structures, and magnetic properties of double perovskites SrLaNiOsO6 and BaLaNiOsO6
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$B a_{2} NiOs O_{6}$ : A Dirac-Mott insulator with ferromagnetism near 100 K
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Synthesis, structure, and magnetic properties of novel B-site ordered double perovskites, SrLaMReO ₆ (M = Mg, Mn, Co and Ni)
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‘A’ cation control of perovskite properties
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