Temperature Dependence of Ion Irradiation Induced Amorphisation of Zirconolite

Abstract

Zirconolite is one of the major host phases for actinides in various wasteforms for immobilizing high level radioactive waste (HLW). Over time, zirconolite's crystalline matrix is damaged by {alpha}-particles and energetic recoil nuclei recoil resulting from {alpha}-decay events. The cumulative damage caused by these particles results in amorphization. Data from natural zirconolites suggest that radiation damage anneals over geologic time and is dependant on the thermal history of the material. Proposed HLW containment strategies rely on both a suitable wasteform and geologic isolation. Depending on the waste loading, depth of burial, and the repository-specific geothermal gradient, burial could result in a wasteform being exposed to temperatures of between 100--450 C. Consequently, it is important to assess the effect of temperature on radiation damage in synthetic zirconolite. Zirconolite containing wasteforms are likely to be hot pressed at or below 1,473 K (1,200 C) and/or sintered at or below 1,623 K (1,350 C). Zirconolite fabricated at temperatures below 1,523 K (1,250 C) contains many stacking faults. As there have been various attempts to link radiation resistance to structure, the authors decided it was also pertinent to assess the role of stacking faults in radiation resistance. In this study, they simulate {alpha}-decay damage in two zirconolite samples by irradiating them with 1.5 MeV Kr{sup +} ions using the High Voltage Electron Microscope-Tandem User Facility (HTUF) at Argonne National Laboratory (ANL) and measure the critical dose for amorphization (D{sub c}) at several temperatures between 20 and 773 K. One of the samples has a high degree of crystallographic perfection, the other contains many stacking faults on the unit cell scale. Previous authors proposed a model for estimating the activation energy of self annealing in zirconolite and for predicting the critical dose for amorphization at any temperature. The authors discuss their results and earlier published data in relation to that model.