Gold in the layered structures of R3Au7Sn3: From relativity to versatility

Provino, Alessia; Steinberg, Simon Alexander; Smetana, Volodymyr; Paramanik, Uday; Manfrinetti, Pietro; Dhar, Sudesh Kumar; Mudring, Anja -Verena

doi:10.1021/acs.cgd.6b00478

Gold in the layered structures of R₃Au₇Sn₃: From relativity to versatility

Journal Article · Mon Jul 11 00:00:00 EDT 2016 · Crystal Growth and Design

DOI:https://doi.org/10.1021/acs.cgd.6b00478· OSTI ID:1321907

Provino, Alessia ^[1]; Steinberg, Simon Alexander ^[2]; Smetana, Volodymyr ^[2]; Paramanik, Uday ^[3]; Manfrinetti, Pietro ^[2]; Dhar, Sudesh Kumar ^[1]; Mudring, Anja -Verena ^[3]

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)

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; P6_3/m, a = 8.110-8.372 Å, c = 9.351-9.609 Å, V_cell = 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 T_N of 13 K for Tb₃Au₇Sn₃. In Ce₃Au₇Sn₃, which has a T_N 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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1321907

Report Number(s):: IS-J--8960

Journal Information:: Crystal Growth and Design, Journal Name: Crystal Growth and Design; ISSN 1528-7483

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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complex intermetallics
electronic structure calculations
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strongly correlated materials