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Two isostructural layered oxohalide compounds containing Mn2+, Te4+ and Si4+; crystal structure and magnetic susceptibility
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
2014 (English)In: Journal of Solid State Chemistry, ISSN 0022-4596, E-ISSN 1095-726X, Vol. 218, 6-9 p.Article in journal (Refereed) Published
Abstract [en]

The new compounds Mn-4(TeO3)(SiO4)X-2 (X=Br, Cl) were synthesized by solid state reactions in sealed evacuated silica tubes. The compounds crystallize in the monoclinic space group P2(1)/m with the unit cell parameters a=5.5463(3) angstrom (5.49434(7) angstrom), b= 6.4893(4) angstrom (6.44184(9) angstrom), c=12.8709(7) A (12.60451 (18) angstrom), beta=93.559(5)degrees (94.1590(12)degrees) and Z=2 for the respective Br and Cl analogues. Manganese adopts various distorted coordination polyhedra; [MnO6] octahedra, [MnO5] tetragonal pyramids and [MnO2X2] tetrahedra. Other building blocks are [SiO4] tetrahedra and [TeO3] trigonal pyramids. The structure is made up from layers having no net charge that are connected via weak Van der Waal interactions. The layers that are parallel to (1 1 0) consist of two manganese oxide sheets which are separated by [Siad tetrahedra. On the outer sides of the sheets are the [MnO2X2] tetrahedra and the [TeO3] trigonal pyramids connected so that the halide ions and the stereochemically active lone pairs on the tellurium atoms protrude from the layers. Magnetic susceptibility measurements reveal a Curie law with a Weiss temperature of theta=-153(3) K for temperatures >= 100 K and indicate antiferromagnetic ordering at TN similar to 4 K. Possible structural origins of the large frustration parameter of f=38 are discussed.

Place, publisher, year, edition, pages
2014. Vol. 218, 6-9 p.
Keyword [en]
Oxohalide, Layered compounds, Crystal structure, Magnetic susceptibility
National Category
Inorganic Chemistry
Research subject
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:su:diva-107092DOI: 10.1016/j.jssc.2014.05.027ISI: 000339987000002OAI: oai:DiVA.org:su-107092DiVA: diva2:743974
Note

AuthorCount:3;

Available from: 2014-09-05 Created: 2014-09-03 Last updated: 2017-12-05Bibliographically approved
In thesis
1. The Role of Tetrahedral Building Blocks in Low-Dimensional Oxohalide Materials
Open this publication in new window or tab >>The Role of Tetrahedral Building Blocks in Low-Dimensional Oxohalide Materials
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The structural architecture found in low-dimensional materials can lead to a number of interesting physical properties including anisotropic conductivity, magnetic frustration and non-linear optical properties. There is no standard synthesis concept described thus far to apply when searching for new low-dimensional compounds, and therefore control on the design of the new materials is of great importance.This thesis describes the synthesis, crystal structure and characterization of some new transition metal oxohalide compounds containing p-elements having a stereochemically active lone-pair. First row transition metal cations have been used in combination with SeIV, SbIII and TeIV ions as lone-pair elements and Cl- and Br- as halide ions. The lone-pairs do not participate in covalent bonding and are responsible for an asymmetric one-sided coordination. Lone-pair elements in combination with halide ions have shown to be powerful structural spacers that can confine transition metal building blocks into low-dimensional arrangements. The halide ions and lone-pairs reside in non-bonded crystal volumes where they interact through weak van der Waals forces. The transition metal atoms are most often arranged to form sheets, chains or small clusters; most commonly layered compounds are formed.To further explore the chemical system and to separate the transition metal entities even more the possibility to include tetrahedral building blocks such as phosphate-, silicate-, sulphate- and vanadate building blocks into this class of compounds has been investigated. Tetrahedral building blocks are well known for their ability of segmenting structural arrangements by corner sharing, which often leads to the formation of open framework structures. The inclusion of tetrahedral building blocks led to the discovery of interesting structural features such as complex hydrogen bonding, formation of unusual solid solutions or faulted stacking of layers.Compounds for which phase pure material could be synthesized have been characterized in terms of their magnetic properties. Most compounds were found to have antiferromagnetic spin interactions and indications of magnetic frustration could be observed in some of them.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry (MMK), Stockholm University, 2014. 60 p.
Keyword
Lone-pair elements, crystal structure, low-dimensional compounds, oxohalides
National Category
Inorganic Chemistry
Research subject
Inorganic Chemistry
Identifiers
urn:nbn:se:su:diva-108160 (URN)978-91-7649-014-3 (ISBN)
Public defence
2014-11-13, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockhom, 13:00 (English)
Opponent
Supervisors
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 6: Manuscript. Paper 9: Manuscript. Paper 10: Manuscript.

Available from: 2014-10-22 Created: 2014-10-13 Last updated: 2014-11-18Bibliographically approved

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