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1.
Sci Rep ; 10(1): 4717, 2020 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-32170108

RESUMO

High entropy alloys (HEA) are an unusual class of materials where mixtures of elements are stochastically arrayed on a simple crystalline lattice. These systems exhibit remarkable functionality, often along several distinct axes: e.g., the examples [TaNb]1-x(TiZrHf)x are high strength and damage resistant refractory metals that also exhibit superconductivity with large upper critical fields. Here we report the discovery of an f-electron containing HEA, [TaNb]0.31(TiUHf)0.69, which is the first to include an actinide ion. Similar to the Zr-analogue, this material crystallizes in a body-centered cubic lattice with the lattice constant a = 3.41(1) Å and exhibits phonon mediated superconductivity with a transition temperatures Tc ≈ 3.2 K and upper critical fields Hc2 ≈ 6.4 T. These results expand this class of materials to include actinide elements, shows that superconductivity is robust in this sub-group, and opens the path towards leveraging HEAs as functional waste forms for a variety of radioisotopes.

2.
J Phys Condens Matter ; 31(16): 165601, 2019 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-30645978

RESUMO

We report on synthesis and characterization of the compounds A 6W4Al43 (A = U and Pu), that form in the hexagonal Ho6Mo4Al43 caged-structure family. The A ions reside within W/Al cages where the A-A nearest neighbors form dimers between adjacent W/Al cages, with U-U and Pu-Pu distances of 3.3892 [Formula: see text] and 3.4080 [Formula: see text], respectively. While the W/Al networks provide environments similar to those of other cage-like materials (e.g. filled skutterudites), the atomic displacement parameters from single crystal x-ray diffraction measurements show that the A-ions do not exhibit rattling behavior. We find that there is site interchange disorder on one of the W/Al sites. Magnetic susceptibility measurements show that U6W4Al43 displays anisotropic Curie-Weiss behavior where it fits to the data yield an effective magnetic moment near 2.0 [Formula: see text]/U. At low temperatures the magnetic susceptibility deviates from the Curie-Weiss temperature dependence and eventually saturates to a constant value. In contrast, Pu6W4Al43 displays nearly temperature independent Pauli paramagnetism for all temperatures, as would be expected if the 5f -electrons are delocalized. The electrical resistivity for U6W4Al43 increases slightly with the decreasing temperature, suggesting that it is dominated by f -electronic hybridization effects and disorder scattering that originates from the W/Al site interchange. Specific heat measurements for U6W4Al43 further reveal an enhanced electronic Sommerfeld coefficient that is consistent with a moderately enhanced charge carrier effective mass. Together these measurements expose these materials as hosts for unstable f -electron magnetism, where the novel cage-like structures control the phenomena through the spacing between the A ions. Through this combination of mild magnetism, the low cost elements of the Al-W cages, and chemical tunability that has been shown for related materials in the same structure, the A 6W4Al43 compounds emerge as promising nuclear waste-forms for transuranics, while the wider family of materials makes an appealing environment for studying f -electron physics in a novel structure.

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