Swift heavy ion induced differential sublattice response to radiation in delta-Sc4Hf3O12
Résumé
Various binary and ternary mixed oxides of actinides, used or occurring in nuclear technology, experience harsh environments of radiation and high temperature leading to phase transformations. These transformations result in changes in their thermophysical and functional properties. Phase stability and radiation-induced transformations in these actinide oxide systems seem primarily governed by the interplay between the different spatial correlations of the anion and cation sublattices, affecting their ability to dissipate the energy deposited by impinging or recoiling ions. Surrogate phases like A4B3O12, A2B5O13, and A2B7O17 (A=Sc and B=Hf or Zr), existing as equilibrium phases in scandium sesquioxide – hafnium/zirconium dioxide pseudo binary systems, offer a non-radioactive playground to explore and understand these complex phase transformations, owing to resemblances in the crystal chemistry leading to specific arrangements of anion and cation sublattices. The current presentation will discuss the radiation response of Sc4Hf3O12 (delta-phase) irradiated by 92 MeV Xe swift heavy ions (SHI). Using quantitative x-ray diffraction and transmission electron microscopy we show that, while a higher fluence of radiation induces a phase transformation from ordered rhombohedral to long-range disordered defect fluorite structure, the immediate response of the anion sublattice is to induce another phase transformation quenching a short-range ordered phase which can be indexed to anion excess bixbyite. This and previously observed phase transformations in other A4B3O12 and A6B1O12 delta-phases will be discussed in light of their polyhedral arrangements that can be correlated with the ion radii variance of A and B cations.