Irradiation-induced defect formation and damage accumulation in single crystal CeO₂

Here, the accumulation of irradiation-induced disorder in single crystal CeO₂ has been investigated over a wide range of ion fluences. Room temperature irradiations of epitaxial CeO₂ thin films using 2 MeV Au²⁺ ions were carried out up to a total fluence of 1.3 x 10¹⁶ cm^–2 Post-irradiation disorder was characterized using ion channeling Rutherford backscattering spectrometry (RBS/C) and confocal Raman spectroscopy. The Raman measurements were interpreted by means of a phonon confinement model, which employed rigid ion calculations to determine the phonon correlation length in the irradiated material. Comparison between the dose dependent changes in correlation length of the Raman measurements and the Ce disorder fraction from RBS/C provides complementary quantitative details on the rate of point and extended defect formation on the Ce and O sub-lattices over a broad range of ion fluences. Raman measurements, which are significantly more sensitive than RBS/C at low doses, reveal that the nucleation rate of defects is highest below 0.1 displacements per atom (dpa). Comparison between Raman and RBS/C measurements suggests that between 0.1 and 10 dpa the damage evolution is characterized by modest growth of point defects and/or small clusters, while above 10 dpa the preexisting defects rapidly grow into extended clusters and/or loops.