Gold in the layered structures of R3Au7Sn3: From relativity to versatility
Abstract
A new isotypic series of ternary rare earth element-gold-tetrel intermetallic compounds has been synthesized and their structures and properties have been characterized. R3Au7Sn3 (R = Y, La-Nd, Sm, Gd-Tm, Lu) crystallize with the hexagonal Gd3Au7Sn3 prototype (Pearson symbol hP26; P63/m, a = 8.110-8.372 Å, c = 9.351-9.609 Å, Vcell = 532.7-583.3 Å3, Z = 2), an ordered variant of the Cu10Sn3-type. Their structure is built up by GdPt2Sn-type layers, which feature edge-sharing Sn@Au6 trigonal antiprisms connected by trigonal R3 groups. Additional insertion of gold atoms leads to the formation of new homoatomic Au clusters, Au@Au6; alternatively, the structure can be considered as a superstructural polyhedral packing of the ZrBeSi-type. The magnetization, heat ca-pacity and electrical resistivity have been measured for R3Au7Sn3 (R = Ce, Pr, Nd and Tb). All four compounds order antiferromagnetically with the highest TN of 13 K for Tb3Au7Sn3. In Ce3Au7Sn3, which has a TN of 2.9 K, the heat capacity and electrical resistivity data in zero and applied fields indicate the presence of Kondo interactions. The coefficient of the linear term in the electronic heat capacity, γ, derived from the heat capacity data below 0.5 K is 211 mJ/Ce mol K2 suggesting strong electronic correlations duemore »
- Authors:
-
- Ames Lab. and Iowa State Univ., Ames, IA (United States); Univ. of Genova, Genova (Italy); Institute SPIN-CNR, Genova (Italy)
- Ames Lab. and Iowa State Univ., Ames, IA (United States)
- T.I.F.R., Mumbai (India)
- Publication Date:
- Research Org.:
- Ames Lab., Ames, IA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1321907
- Report Number(s):
- IS-J-8960
Journal ID: ISSN 1528-7483
- Grant/Contract Number:
- AC02-07CH11358
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Crystal Growth and Design
- Additional Journal Information:
- Journal Name: Crystal Growth and Design; Journal ID: ISSN 1528-7483
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; complex intermetallics; gold clusters; Kondo interaction; strongly correlated materials; electronic structure calculations
Citation Formats
Provino, Alessia, Steinberg, Simon Alexander, Smetana, Volodymyr, Paramanik, Uday, Manfrinetti, Pietro, Dhar, Sudesh Kumar, and Mudring, Anja -Verena. Gold in the layered structures of R3Au7Sn3: From relativity to versatility. United States: N. p., 2016.
Web. doi:10.1021/acs.cgd.6b00478.
Provino, Alessia, Steinberg, Simon Alexander, Smetana, Volodymyr, Paramanik, Uday, Manfrinetti, Pietro, Dhar, Sudesh Kumar, & Mudring, Anja -Verena. Gold in the layered structures of R3Au7Sn3: From relativity to versatility. United States. https://doi.org/10.1021/acs.cgd.6b00478
Provino, Alessia, Steinberg, Simon Alexander, Smetana, Volodymyr, Paramanik, Uday, Manfrinetti, Pietro, Dhar, Sudesh Kumar, and Mudring, Anja -Verena. Mon .
"Gold in the layered structures of R3Au7Sn3: From relativity to versatility". United States. https://doi.org/10.1021/acs.cgd.6b00478. https://www.osti.gov/servlets/purl/1321907.
@article{osti_1321907,
title = {Gold in the layered structures of R3Au7Sn3: From relativity to versatility},
author = {Provino, Alessia and Steinberg, Simon Alexander and Smetana, Volodymyr and Paramanik, Uday and Manfrinetti, Pietro and Dhar, Sudesh Kumar and Mudring, Anja -Verena},
abstractNote = {A new isotypic series of ternary rare earth element-gold-tetrel intermetallic compounds has been synthesized and their structures and properties have been characterized. R3Au7Sn3 (R = Y, La-Nd, Sm, Gd-Tm, Lu) crystallize with the hexagonal Gd3Au7Sn3 prototype (Pearson symbol hP26; P63/m, a = 8.110-8.372 Å, c = 9.351-9.609 Å, Vcell = 532.7-583.3 Å3, Z = 2), an ordered variant of the Cu10Sn3-type. Their structure is built up by GdPt2Sn-type layers, which feature edge-sharing Sn@Au6 trigonal antiprisms connected by trigonal R3 groups. Additional insertion of gold atoms leads to the formation of new homoatomic Au clusters, Au@Au6; alternatively, the structure can be considered as a superstructural polyhedral packing of the ZrBeSi-type. The magnetization, heat ca-pacity and electrical resistivity have been measured for R3Au7Sn3 (R = Ce, Pr, Nd and Tb). All four compounds order antiferromagnetically with the highest TN of 13 K for Tb3Au7Sn3. In Ce3Au7Sn3, which has a TN of 2.9 K, the heat capacity and electrical resistivity data in zero and applied fields indicate the presence of Kondo interactions. The coefficient of the linear term in the electronic heat capacity, γ, derived from the heat capacity data below 0.5 K is 211 mJ/Ce mol K2 suggesting strong electronic correlations due to the Kondo interaction. The electronic structure calculations based on the projector augmented wave method for particular representatives of the series suggest different tendencies of the localized R-4f AOs to hybridize with the valence states. LMTO-based bonding analysis on the non-magnetic La3Au7Sn3 indicates that the integrated crystal orbital Hamilton popu-lations (COHPs) are dominated by the heteroatomic Au–Sn contacts; however, contributions from La–Au and La–Sn separations are significant, both together exceeding 40 % in the overall bonding. Furthermore, homoatomic Au–Au interactions are evident for the Au@Au6 units but, despite of the high atomic concentration of Au in the compound, they do not dominate the entire bonding picture.},
doi = {10.1021/acs.cgd.6b00478},
journal = {Crystal Growth and Design},
number = ,
volume = ,
place = {United States},
year = {Mon Jul 11 00:00:00 EDT 2016},
month = {Mon Jul 11 00:00:00 EDT 2016}
}
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