Some example applications are presented, in which the peculiar Raman fingerprint of PuO₂ can be used for the detection of crystalline Pu⁴⁺ with cubic symmetry in an oxide environment in various host materials, like mixed oxide fuels, inert matrices and corium sub-systems. The PuO₂ Raman fingerprint was previously observed to consist of one main T_2g vibrational mode at 478 cm⁻¹ and two crystal electric field transition lines at 2130 cm⁻¹ and 2610 cm⁻¹. This particular use of Raman spectroscopy is promising for applications in nuclear waste management, safety and safeguard.

The physical and chemical properties at low temperatures of hexavalent disodium neptunate α-Na₂NpO₄ are investigated for the first time in this work using Mössbauer spectroscopy, magnetization, magnetic susceptibility, and heat capacity measurements. The Np(VI) valence state is confirmed by the isomer shift value of the Mössbauer spectra, and the local structural environment around the neptunium cation is related to the fitted quadrupole coupling constant and asymmetry parameters. Moreover, magnetic hyperfine splitting is reported below 12.5 K, which could indicate magnetic ordering at this temperature. This interpretation is further substantiated by the existence of a λ-peak at 12.5 K in the heat capacity curve, which is shifted to lower temperatures with the application of a magnetic field, suggesting antiferromagnetic ordering. However, the absence of any anomaly in the magnetization and magnetic susceptibility data shows that the observed transition is more intricate. In addition, the heat capacity measurements suggest the existence of a Schottky-type anomaly above 15 K associated with a low-lying electronic doublet found about 60 cm^-1 above the ground state doublet. The possibility of a quadrupolar transition associated with a ground state pseudoquartet is thereafter discussed. The present results finally bring new insights into the complex magnetic and electronic peculiarities of α-Na₂NpO₄.