Monazite-Type SmPO 4 as Potential Nuclear Waste Form: Insights into Radiation Effects from Ion-Beam Irradiation and Atomistic Simulations.

Single-phase monazite-type ceramics are considered as potential host matrices for the conditioning of separated plutonium and minor actinides. Sm-orthophosphates were synthesised and their behaviour under irradiation was investigated with respect to their long-term performance in the repository environment. Sintered SmPO 4 pellets and thin lamellae were irradiated with 1, 3.5, and 7 MeV Au ions, up to fluences of 5.1 × 10 14 ions cm -2 to simulate ballistic effects of recoiling nuclei resulting from α -decay of incorporated actinides. Threshold displacement energies for monazite-type SmPO 4 subsequently used in SRIM/TRIM simulations were derived from atomistic simulations. Raman spectra obtained from irradiated lamellae revealed vast amorphisation at the highest fluence used, although local annealing effects were observed. The broadened, but still discernible, band of the symmetrical stretching vibration in SmPO 4 and the negligible increase in P-O bond lengths suggest that amorphisation of monazite is mainly due to a breaking of L n -O bonds. PO 4 groups show structural disorder in the local environment but seem to behave as tight units. Annealing effects observed during the irradiation experiment and the distinctively lower dose rates incurred in actinide bearing waste forms and potential α -radiation-induced annealing effects indicate that SmPO 4 -based waste forms have a high potential for withstanding amorphisation.