Raman spectroscopy for the characterization of defective spent nuclear fuels during interim storage in pools

A specific signature characteristic of irradiation damages in uranium dioxide, the most used nuclear fuel, referred as 'triplet defect bands' has recently been evidenced by Raman Spectroscopy. The objective of this study is to determine how this signature can be used to characterize actual spent nuclear fuel stored in pools. For that purpose, three separate effect studies were carried out. Firstly, an electron irradiation experiment shows that the triplet defect bands are due to ballistic interactions and result from the formation displacements in the uranium sub-lattice. Post electron irradiation, the enhanced oxidation of UO₂ samples is observed and attributed to the migration of irradiation induced oxygen vacancies towards the surface. The formation kinetics of the triplet defect bands in UO₂ when exposed to an inert (Ar) and a reactive (aerated water) contact medium is then investigated through the use of an in-situ Raman installation. Both kinetics can be fitted using a direct impact model, but with different numerical values. Finally, to simulate actual spent nuclear fuels in laboratory conditions, the study of different mixed oxide compounds shows that chemical doping impacts the apparition of the Raman triplet defect bands. The experimental results obtained in this work will be used as complementary data for the interpretation of Raman results of actual defective spent nuclear fuels stored in pool conditions. (author)