Nonequivalent Spin Exchanges of the Hexagonal Spin Lattice Affecting the Low-Temperature Magnetic Properties of RInO3 (R = Gd, Tb, Dy): Importance of Spin–Orbit Coupling for Spin Exchanges between Rare-Earth Cations with Nonzero Orbital Moments

doi:10.1021/acs.inorgchem.8b01274

Title: Nonequivalent Spin Exchanges of the Hexagonal Spin Lattice Affecting the Low-Temperature Magnetic Properties of RInO₃ (R = Gd, Tb, Dy): Importance of Spin–Orbit Coupling for Spin Exchanges between Rare-Earth Cations with Nonzero Orbital Moments

Abstract

Here, rare-earth indium oxides RInO₃ (R = Gd, Tb, Dy) consist of spin-frustrated hexagonal spin lattices made up of rare-earth ions R³⁺, where R³⁺ = Gd³⁺ (f⁷, L = 0), Tb³⁺ (f⁸, L = 3), and Dy³⁺ (f⁹, L = 5). We carried out DFT calculations for RInO₃, including on-site repulsion U with/without spin–orbit coupling (SOC), to explore if their low-temperature magnetic properties are related to the two nonequivalent nearest-neighbor (NN) spin exchanges of their hexagonal spin lattices. Our DFT + U + SOC calculations predict that the orbital moments of the Tb³⁺ and Dy³⁺ ions are smaller than their free-ion values by ~2μ_B while the Tb³⁺ spins have an inplane magnetic anisotropy, in agreement with the experiments. This suggests that the f orbitals of each R³⁺ (R = Tb, Dy) ion are engaged, though weakly, in bonding with the surrounding ligand atoms. The magnetic properties of GdInO₃ with the zero orbital moment are adequately described by the spin exchanges extracted by DFT + U calculations. In describing the magnetic properties of TbInO₃ and DyInO₃ with nonzero orbital moments, however, the spin exchanges extracted by DFT + U + SOC calculations are necessary.

Authors:

Gordon, Elijah E. ^[1]; Cheng, Xiyue ^[2]; Kim, Jaewook ^[3]; Cheong, Sang -Wook ^[3];

^[2];

^[4]

North Carolina State Univ., Raleigh, NC (United States)
Chinese Academy of Sciences (CAS), Fuzhou (China)
Rutgers Univ., Piscataway, NJ (United States)
North Carolina State Univ., Raleigh, NC (United States); Chinese Academy of Sciences (CAS), Fuzhou (China)

Publication Date:: 2018-07-23

Research Org.:: Rutgers Univ., Piscataway, NJ (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1461270

Grant/Contract Number:: FG02-07ER46382

Resource Type:: Accepted Manuscript

Journal Name:: Inorganic Chemistry

Additional Journal Information:: Journal Volume: 57; Journal Issue: 15; Journal ID: ISSN 0020-1669

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats


                    Gordon, Elijah E., Cheng, Xiyue, Kim, Jaewook, Cheong, Sang -Wook, Deng, Shuiquan, and Whangbo, Myung -Hwan. Nonequivalent Spin Exchanges of the Hexagonal Spin Lattice Affecting the Low-Temperature Magnetic Properties of RInO3 (R = Gd, Tb, Dy): Importance of Spin–Orbit Coupling for Spin Exchanges between Rare-Earth Cations with Nonzero Orbital Moments.  United States: N. p., 2018. 
        Web.  doi:10.1021/acs.inorgchem.8b01274.

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                    Gordon, Elijah E., Cheng, Xiyue, Kim, Jaewook, Cheong, Sang -Wook, Deng, Shuiquan, & Whangbo, Myung -Hwan. Nonequivalent Spin Exchanges of the Hexagonal Spin Lattice Affecting the Low-Temperature Magnetic Properties of RInO3 (R = Gd, Tb, Dy): Importance of Spin–Orbit Coupling for Spin Exchanges between Rare-Earth Cations with Nonzero Orbital Moments.  United States.  doi:10.1021/acs.inorgchem.8b01274.

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                    Gordon, Elijah E., Cheng, Xiyue, Kim, Jaewook, Cheong, Sang -Wook, Deng, Shuiquan, and Whangbo, Myung -Hwan. Mon .  
        "Nonequivalent Spin Exchanges of the Hexagonal Spin Lattice Affecting the Low-Temperature Magnetic Properties of RInO3 (R = Gd, Tb, Dy): Importance of Spin–Orbit Coupling for Spin Exchanges between Rare-Earth Cations with Nonzero Orbital Moments".  United States.  doi:10.1021/acs.inorgchem.8b01274.  https://www.osti.gov/servlets/purl/1461270.

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@article{osti_1461270,

  title        = {Nonequivalent Spin Exchanges of the Hexagonal Spin Lattice Affecting the Low-Temperature Magnetic Properties of RInO3 (R = Gd, Tb, Dy): Importance of Spin–Orbit Coupling for Spin Exchanges between Rare-Earth Cations with Nonzero Orbital Moments},

  author       = {Gordon, Elijah E. and Cheng, Xiyue and Kim, Jaewook and Cheong, Sang -Wook and Deng, Shuiquan and Whangbo, Myung -Hwan},

  abstractNote = {Here, rare-earth indium oxides RInO3 (R = Gd, Tb, Dy) consist of spin-frustrated hexagonal spin lattices made up of rare-earth ions R3+, where R3+ = Gd3+ (f7, L = 0), Tb3+ (f8, L = 3), and Dy3+ (f9, L = 5). We carried out DFT calculations for RInO3, including on-site repulsion U with/without spin–orbit coupling (SOC), to explore if their low-temperature magnetic properties are related to the two nonequivalent nearest-neighbor (NN) spin exchanges of their hexagonal spin lattices. Our DFT + U + SOC calculations predict that the orbital moments of the Tb3+ and Dy3+ ions are smaller than their free-ion values by ~2μB while the Tb3+ spins have an inplane magnetic anisotropy, in agreement with the experiments. This suggests that the f orbitals of each R3+ (R = Tb, Dy) ion are engaged, though weakly, in bonding with the surrounding ligand atoms. The magnetic properties of GdInO3 with the zero orbital moment are adequately described by the spin exchanges extracted by DFT + U calculations. In describing the magnetic properties of TbInO3 and DyInO3 with nonzero orbital moments, however, the spin exchanges extracted by DFT + U + SOC calculations are necessary.},

  doi          = {10.1021/acs.inorgchem.8b01274},

  journal      = {Inorganic Chemistry},

  number       = 15,

  volume       = 57,

  place        = {United States},

  year         = {2018},

  month        = {7}

}

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DOI: 10.1021/acs.inorgchem.8b01274

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Figure 1: Essential features of the crystal structure of RInO₃: (a) A layer made up of corner-sharing InO₅ trigonal bipyramids, where the blue spheres represent the In atoms. (b) A layer made up of edgesharing RO₆ octahedra, where the red and pink spheres represent the R(1) and R(2) atoms, respectively.more »

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Works referencing / citing this record:

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Abstract

Citation Formats

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