Frustration and Glasslike Character in RIn1–x MnxO3 (R = Tb, Dy, Gd)

Chen, Peng; Holinsworth, Brian S.; O’Neal, Kenneth R.; Luo, Xuan; Topping, Craig V.; Cheong, Sang W.; Singleton, John; Choi, Eun S.; Musfeldt, Janice L.

doi:10.1021/acs.inorgchem.8b01467

Title: Frustration and Glasslike Character in RIn_1–x Mn_xO₃ (R = Tb, Dy, Gd)

Abstract

Here, we bring together ac susceptibility and dc magnetization to uncover the rich magnetic field-temperature behavior of a series of rare earth indium oxides, RInO₃ (R = Tb, Dy, and Gd). The degree of frustration is much larger than expected, particularly in TbInO₃, and the ground states are glasslike with antiferromagnetic tendencies. The activation energy for spin reorientation is low. Chemical substitution with Mn³⁺ ions to form TbIn_1–xMn_xO₃ (x ≤ 0.01) relieves much of the frustration that characterizes the parent compound and slightly enhances the short-range antiferromagnetic order. The phase diagrams developed from this work reveal the rich competition between spin orders and provide an opportunity to compare the dynamics in the RInO₃ and Mn-substituted systems. Finally, these structure–property relations may be useful for understanding magnetism in other geometrically frustrated multiferroics.

Authors:

^[1]; Holinsworth, Brian S. ^[1];

^[1]; Luo, Xuan ^[2]; Topping, Craig V. ^[3]; Cheong, Sang W. ^[2];

^[4]; Choi, Eun S. ^[5];

^[6]

Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Rutgers Univ., Piscataway, NJ (United States). Rutgers Center for Emergent Materials and Dept. of Physics and Astronomy; Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of). Lab. for Pohang Emergent Materials and Dept. of Physics
Univ. of Oxford (United Kingdom). Clarendon Lab., Condensed Matter Physics
Univ. of Oxford (United Kingdom). Clarendon Lab., Condensed Matter Physics; Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry and Dept. of Physics

Publication Date:: 2018-09-28

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1485392

Report Number(s):: LA-UR-18-25203
Journal ID: ISSN 0020-1669

Grant/Contract Number:: 89233218CNA000001

Resource Type:: Accepted Manuscript

Journal Name:: Inorganic Chemistry

Additional Journal Information:: Journal Volume: 57; Journal Issue: 20; 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; 36 MATERIALS SCIENCE; High Magnetic Field Science

Citation Formats


                    Chen, Peng, Holinsworth, Brian S., O’Neal, Kenneth R., Luo, Xuan, Topping, Craig V., Cheong, Sang W., Singleton, John, Choi, Eun S., and Musfeldt, Janice L. Frustration and Glasslike Character in RIn1–x MnxO3 (R = Tb, Dy, Gd).  United States: N. p., 2018. 
Web.  https://doi.org/10.1021/acs.inorgchem.8b01467.

Copy to clipboard


                    Chen, Peng, Holinsworth, Brian S., O’Neal, Kenneth R., Luo, Xuan, Topping, Craig V., Cheong, Sang W., Singleton, John, Choi, Eun S., & Musfeldt, Janice L. Frustration and Glasslike Character in RIn1–x MnxO3 (R = Tb, Dy, Gd).  United States.  https://doi.org/10.1021/acs.inorgchem.8b01467

Copy to clipboard


                    Chen, Peng, Holinsworth, Brian S., O’Neal, Kenneth R., Luo, Xuan, Topping, Craig V., Cheong, Sang W., Singleton, John, Choi, Eun S., and Musfeldt, Janice L. Fri .  
"Frustration and Glasslike Character in RIn1–x MnxO3 (R = Tb, Dy, Gd)".  United States.  https://doi.org/10.1021/acs.inorgchem.8b01467.  https://www.osti.gov/servlets/purl/1485392.

Copy to clipboard


                    
@article{osti_1485392,

  title        = {Frustration and Glasslike Character in RIn1–x MnxO3 (R = Tb, Dy, Gd)},

  author       = {Chen, Peng and Holinsworth, Brian S. and O’Neal, Kenneth R. and Luo, Xuan and Topping, Craig V. and Cheong, Sang W. and Singleton, John and Choi, Eun S. and Musfeldt, Janice L.},

  abstractNote = {Here, we bring together ac susceptibility and dc magnetization to uncover the rich magnetic field-temperature behavior of a series of rare earth indium oxides, RInO3 (R = Tb, Dy, and Gd). The degree of frustration is much larger than expected, particularly in TbInO3, and the ground states are glasslike with antiferromagnetic tendencies. The activation energy for spin reorientation is low. Chemical substitution with Mn3+ ions to form TbIn1–xMnxO3 (x ≤ 0.01) relieves much of the frustration that characterizes the parent compound and slightly enhances the short-range antiferromagnetic order. The phase diagrams developed from this work reveal the rich competition between spin orders and provide an opportunity to compare the dynamics in the RInO3 and Mn-substituted systems. Finally, these structure–property relations may be useful for understanding magnetism in other geometrically frustrated multiferroics.},

  doi          = {10.1021/acs.inorgchem.8b01467},

  journal      = {Inorganic Chemistry},

  number       = 20,

  volume       = 57,

  place        = {United States},

  year         = {2018},

  month        = {9}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1021/acs.inorgchem.8b01467

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 1 work

Citation information provided by
Web of Science

Figures / Tables:

Figure 1: (a) Hexagonal TbInO₃ lattice with space group symmetry P6₃cm. These polar oxides are highly frustrated because of the triangular lattice of rare earth centers. As shown by the shaded InO₅ and TbO₇ polyhedra, the In³⁺ ions are located on 5-fold coordinated trigonal-bipyramidal sites, whereas the rare earth ionsmore »

All figures and tables (5 total)

Save / Share:

Export Metadata

Save to My Library

Works referencing / citing this record:

Field-induced glassy state in disordered cluster antiferromagnets
journal, October 2019

Schmidt, M.; Romitti, M. V.; Magalhaes, S. G.
Journal of Physics: Condensed Matter, Vol. 32, Issue 3
DOI: 10.1088/1361-648x/ab469c

Figures / Tables found in this record:

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

Similar Records in DOE PAGES and OSTI.GOV collections:

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

Journal Article Gordon, Elijah E. ; Cheng, Xiyue ; Kim, Jaewook ; ... - Inorganic Chemistry

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 theirmore »« less
Cited by 2
https://doi.org/10.1021/acs.inorgchem.8b01274

Full Text Available
Spin structure and magnetic frustration in multiferroic RMn{sub 2}O{sub 5} (R=Tb,Ho,Dy)

Journal Article Blake, G R ; Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439 ; Chapon, L C ; ... - Physical Review. B, Condensed Matter and Materials Physics

We have studied the crystal and magnetic structures of the magnetoelectric materials RMn{sub 2}O{sub 5} (R=Tb,Ho,Dy) using neutron diffraction as a function of temperature. All three materials display incommensurate antiferromagnetic ordering below 40 K, becoming commensurate on further cooling. For R=Tb,Ho, a commensurate-incommensurate transition takes place at low temperatures. The commensurate magnetic structures have been solved and are discussed in terms of competing exchange interactions. The spin configuration within the ab plane is essentially the same for each system, and the radius of R determines the sign of the magnetic exchange between adjacent planes. The inherent magnetic frustration in thesemore »« less
https://doi.org/10.1103/PhysRevB.71.214402
Chemical pressure effects on structural, dielectric and magnetic properties of solid solutions Mn{sub 3−x}Co{sub x}TeO{sub 6}

Journal Article Ivanov, S. A. ; Department of Engineering Sciences, Uppsala University, Box 534, SE-751 21 Uppsala ; Mathieu, R., E-mail: roland.mathieu@angstrom.uu.se ; ... - Materials Research Bulletin

Highlights: • Mn{sub 3}TeO{sub 6} and Co{sub 3}TeO{sub 6} are antiferromagnets with corundum related structures. • The structural and magnetic properties of Mn{sub 3−x}Co{sub x}TeO{sub 6} ceramics were investigated. • All compounds adopt the trigonal structure of Mn{sub 3}TeO{sub 6} up to at least x = 2.4. • The antiferromagnetic transition temperature monotonously increases with x. • NPD data evidences the magnetic structure of the Mn{sub 3−x}Co{sub x}TeO{sub 6} ceramics. - Abstract: The effects of Co{sup 2+} doping on the structural, magnetic and dielectric properties of the multiferroic frustrated antiferromagnet Mn{sub 3}TeO{sub 6} have been investigated. Ceramic samples of themore »« less
https://doi.org/10.1016/J.MATERRESBULL.2013.10.016
Divergent effects of static disorder and hole doping in geometrically frustrated {beta}-CaCr{sub 2}O{sub 4}

Journal Article Dutton, S.E., E-mail: siandutton@cantab.ne ; Broholm, C L ; Cava, R J - Journal of Solid State Chemistry

The gallium substituted and calcium deficient variants of geometrically frustrated {beta}-CaCr{sub 2}O{sub 4}, {beta}-CaCr{sub 2-2x}Ga{sub 2x}O{sub 4} (0.02{<=}x{<=}0.25) and {beta}-Ca{sub 1-y}Cr{sub 2}O{sub 4} (0.075{<=}y{<=}0.15), have been investigated by X-ray powder diffraction, magnetization and specific heat measurements. This allows for a direct comparison of the effects, in a geometrically frustrated magnet, of the static disorder that arises from non-magnetic substitution and the dynamic disorder that arises from hole doping. In both cases, disturbing the Cr{sup 3+} lattice results in a reduction in the degree of magnetic frustration. On substitution of Ga, which introduces disorder without creating holes, a gradual release ofmore »« less
https://doi.org/10.1016/j.jssc.2010.05.032
Manipulation of Dy-Mn coupling and ferrielectric phase diagram of DyMn{sub 2}O{sub 5}: The effect of Y substitution of Dy

Journal Article Zhao, Z. Y. ; Wang, Y. L. ; Lin, L. ; ... - Journal of Applied Physics

DyMn{sub 2}O{sub 5} is an extraordinary example in the family of multiferroic manganites and it accommodates both the 4f and 3d magnetic ions with strong Dy-Mn (4f-3d) coupling. The electric polarization origin is believed to arise not only from the Mn spin interactions but also from the Dy-Mn coupling. Starting from proposed scenario on ferrielectricity in DyMn{sub 2}O{sub 5} where the exchange-strictions associated with the Mn{sup 3+}-Mn{sup 4+}-Mn{sup 3+} blocks and Dy{sup 3+}-Mn{sup 4+}-Dy{sup 3+} blocks generate the two ferroelectric sublattices, we perform a set of characterizations on the structure, magnetism, and electric polarization of Dy{sub 1-x}Y{sub x}Mn{sub 2}O{sub 5}more »« less
https://doi.org/10.1063/1.4935137

Similar Records

Title: Frustration and Glasslike Character in RIn1–x MnxO3 (R = Tb, Dy, Gd)

Abstract

Citation Formats

Figures / Tables:

Field-induced glassy state in disordered cluster antiferromagnets journal, October 2019

Title: Frustration and Glasslike Character in RIn_1–x Mn_xO₃ (R = Tb, Dy, Gd)

Field-induced glassy state in disordered cluster antiferromagnets
journal, October 2019