Mahima Gupta

The effect of low temperature proton irradiation in depleted uranium dioxide was examined as a function of fluence. With 2.6 MeV protons, the fluence limit for preserving a good surface quality was found to be relatively low, about 1.4 and 7.0 × 1017 protons/cm2 for single and poly crystalline samples, respectively. Upon increasing the fluence above this threshold, severe surface flaking and disintegration of samples was observed. Based on scanning electron microscopy (SEM) and X-ray diffraction (XRD) observations the causes of surface failure were associated to high H atomic percent at the peak damage region due to low solubility of H in UO2. The resulting lattice stress is believed to exceed the fracture stress of the crystal at the observed fluencies. The oxygen point defects from the displacement damage may hinder the H diffusion and further increase the lattice stress, especially at the peak damage region.

In situ and ex situ transmission electron microscopy observation of small Kr bubbles in both single-crystal and polycrystalline UO2 were conducted to understand the inert gas bubble behavior in oxide nuclear fuel. The bubble size and volume swelling are shown as weak functions of ion dose but strongly depend on the temperature. The Kr bubble formation at room temperature was observed for the first time. The depth profiles of implanted Kr determined by atom probe tomography are in good agreement with the calculated profiles by SRIM, but the measured concentration of Kr is about 1/4 of the calculated concentration. This difference is mainly due to low solubility of Kr in UO2 matrix and high release of Kr from sample surface under irradiation.

In situ and ex situ transmission electron microscopy observation of small Kr bubbles in bothsingle-crystal and polycrystalline UO2 were conducted to understand the inert gas bubblebehavior in oxide nuclear fuel. The bubble size and volume swelling are shown as a weakfunction of ion dose but strongly depend on the temperature. The Kr bubble formation at roomtemperature was observed for the first time. The depth profiles of implanted Kr determined byatom probe tomography are in good agreement with the calculated profiles by SRIM, but themeasured concentration of Kr is about 1/3 of calculated one. This difference is mainly due to lowsolubility of Kr in UO2 matrix, which has been confirmed by both density-functional theorycalculations and chemical equilibrium analysis.

In situ transmission electron microscopy observation of polycrystalline UO2 (with average grain size of about 5 µm) irradiated with Kr ions at 600°C and 800°C was conducted to understand the radiation-induced dislocation evolution under the influence of grain boundaries. The dislocation evolution in the grain interior of polycrystalline UO2 was similar under Kr irradiation at different ion energies and temperatures. As expected, it was characterized by the nucleation and growth of dislocation loops at low irradiation doses, followed by transformation to extended dislocation lines and tangles at high doses. For the first time, a dislocation-denuded zone was observed near a grain boundary in the 1-MeV Kr-irradiated UO2 sample at 800°C. The denuded zone in the vicinity of grain boundary was not found when the irradiation temperature was at 600°C. The suppression of dislocation loop formation near the boundary is likely due to the enhanced interstitial diffusion toward grain boundary at the high temperature.

In situ transmission electron microscopy (TEM) observation of UO2 single crystal irradiated with Kr ions at high temperatures was conducted to understand the dislocation evolution due to high-energy radiation. The dislocation evolution in UO2 single crystal is shown to occur as nucleation and growth of dislocation loops at low-irradiation doses, followed by transformation to extended dislocation segments and networks at high doses, as well as shrinkage and annihilation of some loops and dislocations due to high temperature annealing. Generally the trends of dislocation evolution in UO2 were similar under Kr irradiation at different ion energies and temperatures (150 keV at 600 °C and 1 MeV at 800 °C) used in this work. Interstitial-type dislocation loops with Burgers vector along 〈1 1 0〉 were observed in the Kr-irradiated UO2. The irradiated specimens were denuded of dislocation loops near the surface.

To gain an understanding of gas bubble transport in oxide nuclear fuel, this paper uses polycrystalline CeO2, composed of both nanograins and micrograins, as a surrogate material for UO2. The CeO2 was implanted with 150-keV Kr ions up to a dose of 1 × 1016 ions/cm2 at 600°C. Transmission electron microscopy characterizations of small Kr bubbles in nanograin and micrograin regions were compared. The grain boundary acted as an efficient defect sink, as evidenced by smaller bubbles and a lower bubble density in the nanograin region as compared to the micrograin region.