Nearly Identical but Not Isotypic: Influence of Lanthanide Contraction on Cs2NaLn(PS 4)2 (Ln = La–Nd, Sm, and Gd–Ho)
Abstract
The effect of the lanthanide contraction often results in topological and symmetry changes in compounds with the same compositions as a function of lanthanide cation size. Here we report on the first example of a lanthanide thiophosphate exhibiting a change in the lanthanide cation environment without any topological or symmetry change. A series of new lanthanide thiophosphates with mixed alkali cations was obtained via a flux crystal growth technique using a CsI flux. The obtained compounds Cs2NaLn(PS4)2 (Ln = La–Nd, Sm, Gd–Ho) were grown as large single crystals (~0.1–1 mm3) and characterized using single crystal X-ray diffraction and magnetic susceptibility measurements. Moving across the series, the structural studies revealed a change in the lanthanide coordination environment dependent upon the identity of the lanthanide. Although all compounds in the Cs2NaLn(PS4)2 series crystallize in the same space group and have the same Wyckoff positions of the atoms, a slight size change between Sm3+ and Gd3+ causes a subtle change in coordination number from 9 (for Ln = La–Sm) to 8 (for Ln = Gd–Ho), resulting in two distinct but virtually identical structure types. Ab initio calculations were performed, and the observed experimental trend was corroborated computationally. Magnetic measurements performed on the Cs2NaLn(PS4)2more »
- Authors:
-
[1];
[2];
[1]
- Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemistry and Biochemistry
- Univ. of South Carolina, Columbia, SC (United States). Nuclear Engineering Program; Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. of South Carolina, Columbia, SC (United States). Nuclear Engineering Program
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Hierarchical Waste Form Materials (CHWM); Univ. of South Carolina, Columbia, SC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Energy Research Scientific Computing Center (NERSC)
- OSTI Identifier:
- 1605386
- Alternate Identifier(s):
- OSTI ID: 1775426
- Grant/Contract Number:
- SC0018739; SC0016574
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 59; Journal Issue: 3; 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; Crystal structure; Chemical structure; Lanthanides; Mathematical methods; Cations
Citation Formats
Klepov, Vladislav V., Pace, Kristen A., Breton, Logan S., Kocevski, Vancho, Besmann, Theodore M., and zur Loye, Hans-Conrad. Nearly Identical but Not Isotypic: Influence of Lanthanide Contraction on Cs2NaLn(PS 4)2 (Ln = La–Nd, Sm, and Gd–Ho). United States: N. p., 2020.
Web. doi:10.1021/acs.inorgchem.9b03200.
Klepov, Vladislav V., Pace, Kristen A., Breton, Logan S., Kocevski, Vancho, Besmann, Theodore M., & zur Loye, Hans-Conrad. Nearly Identical but Not Isotypic: Influence of Lanthanide Contraction on Cs2NaLn(PS 4)2 (Ln = La–Nd, Sm, and Gd–Ho). United States. https://doi.org/10.1021/acs.inorgchem.9b03200
Klepov, Vladislav V., Pace, Kristen A., Breton, Logan S., Kocevski, Vancho, Besmann, Theodore M., and zur Loye, Hans-Conrad. Wed .
"Nearly Identical but Not Isotypic: Influence of Lanthanide Contraction on Cs2NaLn(PS 4)2 (Ln = La–Nd, Sm, and Gd–Ho)". United States. https://doi.org/10.1021/acs.inorgchem.9b03200. https://www.osti.gov/servlets/purl/1605386.
@article{osti_1605386,
title = {Nearly Identical but Not Isotypic: Influence of Lanthanide Contraction on Cs2NaLn(PS 4)2 (Ln = La–Nd, Sm, and Gd–Ho)},
author = {Klepov, Vladislav V. and Pace, Kristen A. and Breton, Logan S. and Kocevski, Vancho and Besmann, Theodore M. and zur Loye, Hans-Conrad},
abstractNote = {The effect of the lanthanide contraction often results in topological and symmetry changes in compounds with the same compositions as a function of lanthanide cation size. Here we report on the first example of a lanthanide thiophosphate exhibiting a change in the lanthanide cation environment without any topological or symmetry change. A series of new lanthanide thiophosphates with mixed alkali cations was obtained via a flux crystal growth technique using a CsI flux. The obtained compounds Cs2NaLn(PS4)2 (Ln = La–Nd, Sm, Gd–Ho) were grown as large single crystals (~0.1–1 mm3) and characterized using single crystal X-ray diffraction and magnetic susceptibility measurements. Moving across the series, the structural studies revealed a change in the lanthanide coordination environment dependent upon the identity of the lanthanide. Although all compounds in the Cs2NaLn(PS4)2 series crystallize in the same space group and have the same Wyckoff positions of the atoms, a slight size change between Sm3+ and Gd3+ causes a subtle change in coordination number from 9 (for Ln = La–Sm) to 8 (for Ln = Gd–Ho), resulting in two distinct but virtually identical structure types. Ab initio calculations were performed, and the observed experimental trend was corroborated computationally. Magnetic measurements performed on the Cs2NaLn(PS4)2 (Ln = Ce, Pr, Nd, Gd, and Tb) compounds revealed paramagnetic behavior.},
doi = {10.1021/acs.inorgchem.9b03200},
journal = {Inorganic Chemistry},
number = 3,
volume = 59,
place = {United States},
year = {Wed Jan 22 00:00:00 EST 2020},
month = {Wed Jan 22 00:00:00 EST 2020}
}
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