No abstract

Energetic radiation can cause dramatic changes in the physical and chemical properties of actinide materials, degrading their performance in fission-based energy systems. As advanced nuclear fuels and wasteforms are developed, fundamental understanding of the processes controlling radiation damage accumulation is necessary. Here we report oxidation state reduction of actinide and analogue elements caused by high-energy, heavy ion irradiation and demonstrate coupling of this redox behaviour with structural modifications. ThO 2 , in which thorium is stable only in a tetravalent state, exhibits damage accumulation processes distinct from those of multivalent cation compounds CeO 2 (Ce 3 þ and Ce 4 þ ) and UO 3 (U 4 þ , U 5 þ and U 6 þ ). The radiation tolerance of these materials depends on the efficiency of this redox reaction, such that damage can be inhibited by altering grain size and cation valence variability. Thus, the redox behaviour of actinide materials is important for the design of nuclear fuels and the prediction of their performance.

Response of dielectric crystals: MgO, Al 2 O 3 and Y 3 Al 5 O 12 (YAG) to irradiation with 167 MeV Xe ions decelerating in the electronic stopping regime is studied. Comprehensive simulations demonstrated that despite similar ion energy losses and the initial excitation kinetics of the electronic systems and lattices, significant differences occur among final structures of ion tracks in these materials, supported by experiments. No ion tracks appeared in MgO, whereas discontinuous distorted crystalline tracks of ~2 nm in diameter were observed in Al 2 O 3 and continuous amorphous tracks were detected in YAG. These track structures in Al 2 O 3 and YAG were confirmed by high resolution TEM data. The simulations enabled us to identify recrystallization as the dominant mechanism governing formation of detected tracks in these oxides. We analyzed effects of the viscosity in molten state, lattice structure and difference in the kinetics of metallic and oxygen sublattices at the crystallization surface on damage recovery in tracks.