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Title: Oxygen trapped by rare earth tetrahedral clusters in Nd{sub 4}FeOS{sub 6}: Crystal structure, electronic structure, and magnetic properties

Abstract

Single crystals of Nd{sub 4}FeOS{sub 6} were grown from an Fe–S eutectic solution. Single crystal X-ray diffraction analysis revealed a Nd{sub 4}MnOSe{sub 6}-type structure (P6{sub 3}mc, a=9.2693(1) Å, c=6.6650(1)Å, V=495.94(1) Å{sup 3}, Z=2), featuring parallel chains of face-sharing [FeS{sub 6×1/2}]{sup 4−} trigonal antiprisms and interlinked [Nd{sub 4}OS{sub 3}]{sup 4+} cubane-like clusters. Oxygen atoms were found to be trapped by Nd{sub 4} clusters in the [Nd{sub 4}OS{sub 3}]{sup 4{sub +}} chains. Structural differences among Nd{sub 4}MnOSe{sub 6}-type Nd{sub 4}FeOS{sub 6} and the related La{sub 3}CuSiS{sub 7}− and Pr{sub 8}CoGa{sub 3}-type structures have been described. Magnetic susceptibility measurements on Nd{sub 4}FeOS{sub 6} suggested the dominance of antiferromagnetic interactions at low temperature, but no magnetic ordering down to 2 K was observed. Spin-polarized electronic structure calculations revealed magnetic frustration with dominant antiferromagnetic interactions. - Graphical abstract: Trapping of oxygen in Nd{sub 4} tetrahedral clusters results in the formation of the Nd{sub 4}MnOSe{sub 6}-type Nd{sub 4}FeOS{sub 6}, in contrast to the La{sub 3}CuSiS{sub 7}-type oxygen-free Nd{sub 4}FeS{sub 7} and related Pr{sub 8}CoGa{sub 3}-type structures. Complex magnetic frustration inhibits magnetic ordering at low temperature. - Highlights: • Single crystals of Nd{sub 4}FeOS{sub 6} were grown using self-flux method. • Oxygen was found trapped by Nd{submore » 4} tetrahedral clusters. • Comparison with two closely related structural types were discussed. • Magnetic measurements revealed antiferromagnetic (AFM) interaction. • VASP calculations confirmed strong magnetic frustration in AFM model.« less

Authors:
 [1];  [1];  [2]; ; ; ;  [1];  [1]
  1. Division of Materials Sciences and Engineering, Ames Laboratory, US-DOE, Ames, IA 50011 (United States)
  2. Department of Chemistry, Iowa State University, Ames, IA 50011 (United States)
Publication Date:
OSTI Identifier:
22486751
Resource Type:
Journal Article
Journal Name:
Journal of Solid State Chemistry
Additional Journal Information:
Journal Volume: 229; Other Information: Copyright (c) 2015 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0022-4596
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ANTIFERROMAGNETISM; ATOMIC FORCE MICROSCOPY; COMPARATIVE EVALUATIONS; COPPER SILICIDES; COPPER SULFIDES; CRYSTAL GROWTH; CRYSTAL STRUCTURE; DEUTERIDES; ELECTRONIC STRUCTURE; EUTECTICS; HEXAGONAL LATTICES; IRON OXIDES; IRON SULFIDES; LANTHANUM COMPOUNDS; MAGNETIC SUSCEPTIBILITY; MAGNETIZATION; MONOCRYSTALS; NEODYMIUM COMPOUNDS; SPIN ORIENTATION; X-RAY DIFFRACTION

Citation Formats

Lin, Qisheng, Taufour, Valentin, Department of Physics and Astronomy, Iowa State University, Ames, IA 50011, Zhang, Yuemei, Wood, Max, Drtina, Thomas, Bud’ko, Sergey L., Canfield, Paul C., Department of Physics and Astronomy, Iowa State University, Ames, IA 50011, Miller, Gordon J., and Department of Chemistry, Iowa State University, Ames, IA 50011. Oxygen trapped by rare earth tetrahedral clusters in Nd{sub 4}FeOS{sub 6}: Crystal structure, electronic structure, and magnetic properties. United States: N. p., 2015. Web. doi:10.1016/J.JSSC.2015.05.020.
Lin, Qisheng, Taufour, Valentin, Department of Physics and Astronomy, Iowa State University, Ames, IA 50011, Zhang, Yuemei, Wood, Max, Drtina, Thomas, Bud’ko, Sergey L., Canfield, Paul C., Department of Physics and Astronomy, Iowa State University, Ames, IA 50011, Miller, Gordon J., & Department of Chemistry, Iowa State University, Ames, IA 50011. Oxygen trapped by rare earth tetrahedral clusters in Nd{sub 4}FeOS{sub 6}: Crystal structure, electronic structure, and magnetic properties. United States. https://doi.org/10.1016/J.JSSC.2015.05.020
Lin, Qisheng, Taufour, Valentin, Department of Physics and Astronomy, Iowa State University, Ames, IA 50011, Zhang, Yuemei, Wood, Max, Drtina, Thomas, Bud’ko, Sergey L., Canfield, Paul C., Department of Physics and Astronomy, Iowa State University, Ames, IA 50011, Miller, Gordon J., and Department of Chemistry, Iowa State University, Ames, IA 50011. 2015. "Oxygen trapped by rare earth tetrahedral clusters in Nd{sub 4}FeOS{sub 6}: Crystal structure, electronic structure, and magnetic properties". United States. https://doi.org/10.1016/J.JSSC.2015.05.020.
@article{osti_22486751,
title = {Oxygen trapped by rare earth tetrahedral clusters in Nd{sub 4}FeOS{sub 6}: Crystal structure, electronic structure, and magnetic properties},
author = {Lin, Qisheng and Taufour, Valentin and Department of Physics and Astronomy, Iowa State University, Ames, IA 50011 and Zhang, Yuemei and Wood, Max and Drtina, Thomas and Bud’ko, Sergey L. and Canfield, Paul C. and Department of Physics and Astronomy, Iowa State University, Ames, IA 50011 and Miller, Gordon J. and Department of Chemistry, Iowa State University, Ames, IA 50011},
abstractNote = {Single crystals of Nd{sub 4}FeOS{sub 6} were grown from an Fe–S eutectic solution. Single crystal X-ray diffraction analysis revealed a Nd{sub 4}MnOSe{sub 6}-type structure (P6{sub 3}mc, a=9.2693(1) Å, c=6.6650(1)Å, V=495.94(1) Å{sup 3}, Z=2), featuring parallel chains of face-sharing [FeS{sub 6×1/2}]{sup 4−} trigonal antiprisms and interlinked [Nd{sub 4}OS{sub 3}]{sup 4+} cubane-like clusters. Oxygen atoms were found to be trapped by Nd{sub 4} clusters in the [Nd{sub 4}OS{sub 3}]{sup 4{sub +}} chains. Structural differences among Nd{sub 4}MnOSe{sub 6}-type Nd{sub 4}FeOS{sub 6} and the related La{sub 3}CuSiS{sub 7}− and Pr{sub 8}CoGa{sub 3}-type structures have been described. Magnetic susceptibility measurements on Nd{sub 4}FeOS{sub 6} suggested the dominance of antiferromagnetic interactions at low temperature, but no magnetic ordering down to 2 K was observed. Spin-polarized electronic structure calculations revealed magnetic frustration with dominant antiferromagnetic interactions. - Graphical abstract: Trapping of oxygen in Nd{sub 4} tetrahedral clusters results in the formation of the Nd{sub 4}MnOSe{sub 6}-type Nd{sub 4}FeOS{sub 6}, in contrast to the La{sub 3}CuSiS{sub 7}-type oxygen-free Nd{sub 4}FeS{sub 7} and related Pr{sub 8}CoGa{sub 3}-type structures. Complex magnetic frustration inhibits magnetic ordering at low temperature. - Highlights: • Single crystals of Nd{sub 4}FeOS{sub 6} were grown using self-flux method. • Oxygen was found trapped by Nd{sub 4} tetrahedral clusters. • Comparison with two closely related structural types were discussed. • Magnetic measurements revealed antiferromagnetic (AFM) interaction. • VASP calculations confirmed strong magnetic frustration in AFM model.},
doi = {10.1016/J.JSSC.2015.05.020},
url = {https://www.osti.gov/biblio/22486751}, journal = {Journal of Solid State Chemistry},
issn = {0022-4596},
number = ,
volume = 229,
place = {United States},
year = {Tue Sep 15 00:00:00 EDT 2015},
month = {Tue Sep 15 00:00:00 EDT 2015}
}

Works referencing / citing this record:

Polar Intermetallics Pr 5 Co 2 Ge 3 and Pr 7 Co 2 Ge 4 with Planar Hydrocarbon-Like Metal Clusters
journal, July 2017


A study of the physical properties of single crystalline Fe5B2P
journal, March 2016