Synthesis and properties of A$_x$V$_2$Al$_{20}$ (A = Th, U, Np, Pu) ternary actinide aluminides

TL;DR

This study synthesized and characterized actinide aluminides with a CeCr2Al20-type structure, revealing differences in electronic behavior compared to lanthanide analogs and observing no magnetic order down to 2.5 K.

Contribution

First synthesis and structural analysis of A_xV2Al20 (A = Th, U, Np, Pu) actinide aluminides, highlighting differences in electron localization and itinerancy compared to lanthanide counterparts.

Findings

All compounds crystallize in CeCr2Al20-type structure.

No magnetic ordering observed down to 2.5 K.

Presence of low-energy Einstein mode indicated by specific heat anomalies.

Abstract

Polycrystalline samples of A$_x$V$_2$Al$_{20}$ (A = Ce, Th, U, Np, Pu; 0.7 =< x =< 1.0) actinide intermetallics were synthesized using the arc-melting method. Crystal structure studies were performed by means of powder x-ray diffraction and the Rietveld refinement method. All studied compounds crystallize in the CeCr$_{2}$Al$_{20}$-type structure (space group Fd-3m, no. 227) with the actinide or Ce atom located in the oversized cage formed by Al atoms. Comparison of the crystallographic results with the reported data for LnV$_{2}$Al$_{20}$ (Ln = lanthanoids) counterparts reveals distinctly different behavior of the lanthanide- and actinide-bearing compounds. This difference is suggested to be caused by fairly localized character of the 4f electrons, whereas itinerant character of the 5f electrons is likely seen for U- and Np-containing phases. Magnetic susceptibility and specific heat measurements did not reveal any magnetic ordering in U$_{0.8}$V$_{2}$Al$_{20}$, Np$_{0.8}$V$_{2}$Al$_{20}$ and Pu$_{0.8}$V$_{2}$Al$_{20}$ down to 2.5 K. A small anomaly in low-temperature specific heat of Ce$_{0.8}$V$_{2}$Al$_{20}$, U$_{0.8}$V$_{2}$Al$_{20}$, and Np$_{0.8}$V$_{2}$Al$_{20}$ is observed, likely arising from a low-energy Einstein mode.