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Title: Tunable magnetic order in low-symmetry SeO3 ligand linked TM3(SeO3)3H2O (TM=Mn , Co, and Ni) compounds

Abstract

The ability to design crystal lattices with specific sublattice geometries has long been sought after especially in the context of harnessing magnetic frustration to elicit emergent physics. One approach which has seen some success recently is to design magnetic sublattices chemically through the use of nonmagnetic linker ligands as scaffolding for the magnetic ions. In this work we report the magnetic properties of one such family of materials, the transition metal (TM) selenite hydrates with chemical formula TM3(SeO3)3H2O. These materials link highly distorted TMO6 octahedra via nonmagnetic [SeO3]2+ linkers. Studying members with TM = Mn, Co, and Ni we use magnetic susceptibility and neutron powder diffraction to identify antiferromagnetic order in all three compounds with moderate frustration indexes. A comparison of the magnetic structures suggests that while the overall structure of the SeO3 scaffolding remains unchanged the TM effects changes in the magnetic properties through tuning the internal bonding parameters and the single-ion physics. Changing from Mn to Co is found to be particularly consequential manifesting changes in both the ordered-moment direction and in the direction of the ordering vector. Field-dependent measurements of the susceptibility and heat capacity reveal metamagnetic transitions in both Mn3(SeO3)3H2O and Co3(SeO3)3H2O indicating nearby magnetic groundmore » states accessible under relatively small applied fields. Density functional theory calculations broadly confirm these results, showing both a sensitivity of the magnetic structure to the TM and its local environment. Although no spin liquid behavior is achieved, these results suggest the fruitfulness of such synthesis philosophies and encourage future work to engender higher frustration in these materials via doping, field, pressure, or larger linker ligands.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1731072
Alternate Identifier(s):
OSTI ID: 1600066
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 4; Journal Issue: 2; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; magnetism; metamagnetism; crystal structures; crystal growth; density functional theory; neutron diffraction

Citation Formats

Taddei, Keith, Sanjeewa, Liurukara D., Xing, Jie, Zhang, Qiang, Parker, David S., Podlesnyak, Andrey A., Dela Cruz, Clarina R., and Sefat, Athena Safa. Tunable magnetic order in low-symmetry SeO3 ligand linked TM3(SeO3)3H2O (TM=Mn , Co, and Ni) compounds. United States: N. p., 2020. Web. doi:10.1103/physrevmaterials.4.024410.
Taddei, Keith, Sanjeewa, Liurukara D., Xing, Jie, Zhang, Qiang, Parker, David S., Podlesnyak, Andrey A., Dela Cruz, Clarina R., & Sefat, Athena Safa. Tunable magnetic order in low-symmetry SeO3 ligand linked TM3(SeO3)3H2O (TM=Mn , Co, and Ni) compounds. United States. https://doi.org/10.1103/physrevmaterials.4.024410
Taddei, Keith, Sanjeewa, Liurukara D., Xing, Jie, Zhang, Qiang, Parker, David S., Podlesnyak, Andrey A., Dela Cruz, Clarina R., and Sefat, Athena Safa. Tue . "Tunable magnetic order in low-symmetry SeO3 ligand linked TM3(SeO3)3H2O (TM=Mn , Co, and Ni) compounds". United States. https://doi.org/10.1103/physrevmaterials.4.024410. https://www.osti.gov/servlets/purl/1731072.
@article{osti_1731072,
title = {Tunable magnetic order in low-symmetry SeO3 ligand linked TM3(SeO3)3H2O (TM=Mn , Co, and Ni) compounds},
author = {Taddei, Keith and Sanjeewa, Liurukara D. and Xing, Jie and Zhang, Qiang and Parker, David S. and Podlesnyak, Andrey A. and Dela Cruz, Clarina R. and Sefat, Athena Safa},
abstractNote = {The ability to design crystal lattices with specific sublattice geometries has long been sought after especially in the context of harnessing magnetic frustration to elicit emergent physics. One approach which has seen some success recently is to design magnetic sublattices chemically through the use of nonmagnetic linker ligands as scaffolding for the magnetic ions. In this work we report the magnetic properties of one such family of materials, the transition metal (TM) selenite hydrates with chemical formula TM3(SeO3)3H2O. These materials link highly distorted TMO6 octahedra via nonmagnetic [SeO3]2+ linkers. Studying members with TM = Mn, Co, and Ni we use magnetic susceptibility and neutron powder diffraction to identify antiferromagnetic order in all three compounds with moderate frustration indexes. A comparison of the magnetic structures suggests that while the overall structure of the SeO3 scaffolding remains unchanged the TM effects changes in the magnetic properties through tuning the internal bonding parameters and the single-ion physics. Changing from Mn to Co is found to be particularly consequential manifesting changes in both the ordered-moment direction and in the direction of the ordering vector. Field-dependent measurements of the susceptibility and heat capacity reveal metamagnetic transitions in both Mn3(SeO3)3H2O and Co3(SeO3)3H2O indicating nearby magnetic ground states accessible under relatively small applied fields. Density functional theory calculations broadly confirm these results, showing both a sensitivity of the magnetic structure to the TM and its local environment. Although no spin liquid behavior is achieved, these results suggest the fruitfulness of such synthesis philosophies and encourage future work to engender higher frustration in these materials via doping, field, pressure, or larger linker ligands.},
doi = {10.1103/physrevmaterials.4.024410},
journal = {Physical Review Materials},
number = 2,
volume = 4,
place = {United States},
year = {Tue Feb 18 00:00:00 EST 2020},
month = {Tue Feb 18 00:00:00 EST 2020}
}

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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Long-range antiferromagnetic order in the frustrated XY pyrochlore antiferromagnet Er 2 Ge 2 O 7
journal, February 2014


Local-Ising-type magnetic order and metamagnetism in the rare-earth pyrogermanate Er 2 Ge 2 O 7
journal, January 2019


Spin liquids in frustrated magnets
journal, March 2010


Crystal structures of Co3(SeO3)3�H2O and Ni3(SeO3)3�H2O, two new isotypic compounds
journal, January 1991

  • Wildner, Manfred
  • Monatshefte f�r Chemie Chemical Monthly, Vol. 122, Issue 8-9
  • DOI: 10.1007/BF00811457

Magnetic pyrochlore oxides
journal, January 2010

  • Gardner, Jason S.; Gingras, Michel J. P.; Greedan, John E.
  • Reviews of Modern Physics, Vol. 82, Issue 1
  • DOI: 10.1103/RevModPhys.82.53

Critical behavior of the metallic triangular-lattice Heisenberg antiferromagnet PdCrO 2
journal, March 2009


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


The synthesis and crystal structure of a new nickel selenite hydrate, Ni3(SeO3)3 · H2O
journal, June 1991

  • Mcmanus, Adrian V. P.; Harrison, William T. A.; Cheetham, Anthony K.
  • Journal of Solid State Chemistry, Vol. 92, Issue 2
  • DOI: 10.1016/0022-4596(91)90333-D

A suite-level review of the neutron powder diffraction instruments at Oak Ridge National Laboratory
journal, September 2018

  • Calder, S.; An, K.; Boehler, R.
  • Review of Scientific Instruments, Vol. 89, Issue 9
  • DOI: 10.1063/1.5033906

Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr 4 S 8
journal, April 2018


Spin-Liquid Ground State of the S = 1/2 Kagome Heisenberg Antiferromagnet
journal, April 2011


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


Antiferromagnetic order in the pyrochlores R 2 Ge 2 O 7   ( R = Er , Yb )
journal, October 2015


Magnetic structure and susceptibility of CoSe 2 O 5 : An antiferromagnetic chain compound
journal, July 2010


Two trimeric tri-TiIV-substituted Keggin tungstogermanates based on tetrahedral linkers
journal, November 2008


GSAS-II : the genesis of a modern open-source all purpose crystallography software package
journal, March 2013


Bilbao Crystallographic Server: I. Databases and crystallographic computing programs
journal, January 2006

  • Aroyo, Mois Ilia; Perez-Mato, Juan Manuel; Capillas, Cesar
  • Zeitschrift für Kristallographie - Crystalline Materials, Vol. 221, Issue 1
  • DOI: 10.1524/zkri.2006.221.1.15

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011


Bilbao Crystallographic Server. II. Representations of crystallographic point groups and space groups
journal, March 2006

  • Aroyo, Mois I.; Kirov, Asen; Capillas, Cesar
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 62, Issue 2
  • DOI: 10.1107/S0108767305040286

Quantification of local Ising magnetism in rare-earth pyrogermanates Er 2 Ge 2 O 7 and Yb 2 Ge 2 O 7
journal, January 2020


Simple frustrated systems: chains, strips and squares
journal, December 1978

  • Derrida, B.; Vannimenus, J.; Pomeau, Y.
  • Journal of Physics C: Solid State Physics, Vol. 11, Issue 23
  • DOI: 10.1088/0022-3719/11/23/019

Recent progress on synthesis and structural aspects of rare-earth phosphates
journal, June 2017


On the allowed values for the triclinic unit-cell angles
journal, November 2010

  • Foadi, James; Evans, Gwyndaf
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 67, Issue 1
  • DOI: 10.1107/S0108767310044296

Suppression of the antiferromagnetic metallic state in the pressurized MnB i 2 T e 4 single crystal
journal, September 2019


Classification of topological quantum matter with symmetries
journal, August 2016


Three-Dimensional Organically Templated Open-Framework Transition Metal Selenites
journal, January 2002


Structural and magnetic characterization of the one-dimensional S = 5 / 2 antiferromagnetic chain system SrMn ( V O 4 ) ( OH )
journal, June 2016

  • Sanjeewa, Liurukara D.; Garlea, Vasile O.; McGuire, Michael A.
  • Physical Review B, Vol. 93, Issue 22
  • DOI: 10.1103/PhysRevB.93.224407

Hydrothermal synthesis, crystal structure, spectroscopic and magnetic properties of Mn 4 (H 2 O) 3 (SeO 3 ) 4 and Mn 3 (H 2 O)(SeO 3 ) 3
journal, January 2002

  • Larrañaga, Aitor; Mesa, José L.; Pizarro, José L.
  • J. Chem. Soc., Dalton Trans., Issue 18
  • DOI: 10.1039/B206515K

Synthesis and structural variety of first Mn and Bi selenites and selenite chlorides
journal, March 2019

  • Kovrugin, Vadim M.; Colmont, Marie; Siidra, Oleg I.
  • Zeitschrift für Kristallographie - Crystalline Materials, Vol. 234, Issue 3
  • DOI: 10.1515/zkri-2018-2088

Exchange interactions in insulators and semiconductors
journal, September 1990


Strongly Geometrically Frustrated Magnets
journal, August 1994


Magnetic monopoles in spin ice
journal, January 2008

  • Castelnovo, C.; Moessner, R.; Sondhi, S. L.
  • Nature, Vol. 451, Issue 7174
  • DOI: 10.1038/nature06433

An extreme case of ZnO 6 octahedral distortion in trizinc tris(selenite) hydrate, Zn 3 (SeO 3 ) 3
journal, December 1999

  • Harrison, W. T. A.
  • Acta Crystallographica Section C Crystal Structure Communications, Vol. 55, Issue 12
  • DOI: 10.1107/S0108270199011099

Exotic Magnetic Field-Induced Spin-Superstructures in a Mixed Honeycomb-Triangular Lattice System
journal, February 2019

  • Garlea, V. Ovidiu; Sanjeewa, Liurukara D.; McGuire, Michael A.
  • Physical Review X, Vol. 9, Issue 1
  • DOI: 10.1103/PhysRevX.9.011038