Syntheses, Structure, Magnetism, and Optical Properties of the Ordered Interlanthanide Copper Chalcogenides Ln{sub 2}YbCuQ{sub 5} (Ln = La, Ce, Pr, Nd, Sm; Q = S, Se): Evidence for Unusual Magnetic Ordering in Sm{sub 2}YbCuS{sub 5}
Ln{sub 2}YbCuQ{sub 5} (Ln = La, Ce, Pr, Nd, Sm; Q = S, Se) have been prepared by direct reaction of the elements in Sb{sub 2}Q{sub 3} (Q = S, Se) fluxes at 900 °C. All compounds have been characterized by single-crystal X-ray diffraction methods and they are isotypic. The structure of Ln{sub 2}YbCuQ{sub 5} consists of one-dimensional {sup 1}{sub {infinity}} [YbCuQ{sub 5}]{sup 6-} ribbons extending along the b axis that are connected by larger Ln{sup 3+} ions. Each ribbon is constructed from two single chains of [YbQ{sub 6}] octahedra with one double chain of [CuQ{sub 5}] trigonal bipyramids in the middle. All three chains connect with each other via edge-sharing. There are two crystallographically unique Ln atoms, one octahedral Yb site, and two disordered Cu positions inside of distorted Q{sub 5} trigonal bipyramids. Both Ln atoms are surrounded by eight Q atoms in bicapped trigonal prisms. The magnetic properties of Ln{sub 2}YbCuQ{sub 5} have been characterized using magnetic susceptibility and heat capacity measurements, while their optical properties have been explored using UV-vis-NIR diffuse reflectance spectroscopy. Cesub 2}YbCuSe{sub 5}, La{sub 2}YbCuS{sub 5}, Ce{sub 2}YbCuS{sub 5}, and Pr{sub 2}YbCuS{sub 5} are Curie-Weiss paramagnets. La{sub 2}YbCuSe{sub 5} and Nd{sub 2}YbCuS{sub 5} show evidence for short-range antiferromagnetic ordering at low temperatures. Sm{sub 2}YbCuS{sub 5} shows magnetic ordering at 5.9 K, followed by negative magnetization at low external fields. The band gaps of La{sub 2}YbCuSe{sub 5}, Ce{sub 2}YbCuSe{sub 5}, La{sub 2}YbCuS{sub 5}, Ce{sub 2}YbCuS{sub 5}, Pr{sub 2}YbCuS{sub 5}, Nd{sub 2}YbCuS{sub 5},and Sm{sub 2}YbCuS{sub 5} are 1.15 eV, 1.05 eV, 1.45 eV, 1.37 eV, 1.25 eV, 1.35 eV, and 1.28 eV respectively.
- Research Organization:
- Ernest Orlando Lawrence Berkeley National Laboratory, Berkeley, CA (US)
- Sponsoring Organization:
- Chemical Sciences Division
- DOE Contract Number:
- AC02-05CH11231
- OSTI ID:
- 1051658
- Report Number(s):
- LBNL-5158E
- Journal Information:
- Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 5 Vol. 23; ISSN 0897-4756
- Country of Publication:
- United States
- Language:
- English
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