Anter EL-AZAB

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.

Transmission electron microscopy observation of Kr bubble evolution in polycrystalline UO2 annealed at high temperature was conducted in order to understand the inert gas behavior in oxide nuclear fuel. The average diameter of intragranular bubbles increased gradually from 0.8 nm in as-irradiated sample at room temperature to 2.6 nm at 1600 °C and the bubble size distribution changed from a uniform distribution to a bimodal distribution above 1300 °C. The size of intergranular bubbles increased more rapidly than intragranular ones and bubble denuded zones near grain boundaries formed in all the annealed samples. It was found that high-angle grain boundaries held bigger bubbles than low-angle grain boundaries. Complementary atomistic modeling was conducted to interpret the effects of grain boundary character on the Kr segregation. The area density of strong segregation sites in the high-angle grain boundaries is much higher than that in the low angle grain boundaries.

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.

We present a model to study the electrochemical effects of voids in oxide materials under equilibrium conditions and apply this model to uranium dioxide. Based on thermodynamic arguments, we claim that voids in uranium dioxide must contain oxygen gas at a pressure that we determine via a Kelvin equation in terms of temperature, void radius and the oxygen pressure of the outside gas reservoir in equilibrium with the oxide. The oxygen gas within a void gives rise to ionosorption and the formation of a layer of surface-charge on the void surface,which,in turn, induces an influence zone of space charge into the matrix surrounding the void. Since the space charge is carried in part by atomic defects, it is concluded that, as a part of the thermodynamic equilibrium of oxides containing voids, the off-stoichiometry around the void is different from its remote bulk value. As such,in a uranium dioxide solid with a void ensemble, the average off-stoichiometry level in the material differs from that of the void-free counterpart. The model is applied to isolated voids in off-stoichiometric uranium dioxide for a wide range of temperature and disorder state of the oxide.

During the fission process in a nuclear reactor, uranium dioxide (UO2) fuel material is irradiated, forming fission products (FPs). The addition of FPs alters the path phonons travel in UO2, detrimentally altering the thermal conductivity of the fuel. [1] To improve fuel performance, a fundamental understanding of the role of insoluble FPs, such as Xenon (Xe), during microstructural evolution is critical. Correlative characterization techniques where atom probe tomography (APT) is paired with transmission electron microscopy (TEM) can provide unique insights into the segregation behavior of FPs. Coupling these techniques with computer simulations of fission product distribution provide deeper understanding of FP migration during service. Although there are limitations with each of these techniques in isolation, significant insight into material behavior can be gained with the concurrent and synergistic pairing of multiple experimental and computational techniques.

The microstructural changes and associated effects on thermal conductivity were examined in UO2 after irradiation using 3.9 MeV He2+ ions. Lattice expansion of UO2 was observed in X-ray diffraction after ion irradiation up to 5 × 1016 He2+/cm2 at low-temperature (<200 °C). Transmission electron microscopy (TEM) showed homogenous irradiation damage across an 8 μm thick plateau region, which consisted of small dislocation loops accompanied by dislocation segments. Dome-shaped blisters were observed at the peak damage region (depth around 8.5 μm) in the sample subjected to 5 × 1016 He2+/cm2, the highest fluence reached, while similar features were not detected at 9 × 1015 He2+/cm2. Laser-based thermo-reflectance measurements showed that the thermal conductivity for the irradiated layer decreased about 55% for the high fluence sample and 35% for the low fluence sample as compared to an un-irradiated reference sample. Detailed analysis for the thermal conductivity indicated that the conductivity reduction was caused by the irradiation induced point defects.

In situ Transmission Electron Microscopy was conducted for single crystal UO2 to understand the microstructure evolution during 300 keV Xe irradiation at room temperature. The dislocation microstructure evolution was shown to occur as nucleation and growth of dislocation loops at low irradiation doses, followed by transformation to extended dislocation segments and tangles at higher doses. Xe bubbles with dimensions of 1-2 nm were observed after room-temperature irradiation. Electron Energy Loss Spectroscopy indicated that UO2 remained stoichiometric under room temperature Xe irradiation.

The role of cavities on deformation-induced martensitic phase transformations is studied in a laser-welded and neutron irradiated austenitic stainless steel. Orientation dependent nanoindentation experiments are performed in the base metal and the weld heat affected zone (HAZ) at room temperature. Transmission electron microscopy study of deformed microstructures indicates indentation-induced α’-martensite forms in the base metal, whereas α’- and ε-martensite arise in the HAZ. The different pathway of martensite phase transformation is attributed to the laser weld-induced annealing of cavities. Our results suggest that deformation-induced martensitic phase transformation of austenitic stainless steel is correlated to neutron irradiated cavity structures.