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The structural, elastic, electronic, vibrational and thermodynamic properties of uranium aluminides UAlx (x = 2, 3, 4) were studied by density functional theory calculations. The single crystal elastic constants of UAlx were predicted using the stress-strain method, which were further used to calculate the polycrystalline aggregate properties of UAlx, including bulk modulus, shear modulus, Young’s modulus, and Poisson’s ratio, etc. The calculated electronic density of states confirm that UAlx compounds are metallic phases with majority states at the Fermi level contributed by U 5f electrons. The phonon dispersion relations and density of states show that the low frequency acoustic phonon modes of UAlx are dominated by the lattice vibration of uranium atoms while high frequency optical phonon modes are from the vibration of aluminum atoms. Using quasiharmonic approximation, thermodynamic properties of UAlx, including Gibbs free energy, entropy, heat capacity, and linear thermal expansion coefficient, were predicted by including both lattice vibrational and thermal electronic contributions. The thermal electronic energy was found to be crucial for the description of the temperature dependence of the thermodynamic properties. The derived Gibbs energy functions of UAlx are expected to be useful to the thermodynamic modeling of the ternary U-Mo-Al system.

The evolution of fission gas bubbles in irradiated materials plays a critical role in the microstructural processes that leads to dimensional changes of U-Mo alloy fuels, e.g., fuel swelling. Although the intergranular bubbles-induced fuel swelling has been long-discussed for U-Mo fuel, there are very few computational studies of the formation of intragranular gas bubbles and its impact on fuel swelling. To this end, we develop a three-dimensional phase-field model to investigate the evolution of intragranular gas bubbles in U-Mo fuel. Fission induced defect formation and annihilation processes, such as vacancy-interstitial recombination, fission gas atom resolution, and interactions with dislocations and grain boundaries are incorporated in the model. Simulations show that the intragranular gas bubbles can be stabilized to certain sizes due to the balance between the generation and annihilation of defects. The intragranular gas bubbles induced fuel swelling is predicted to be comparable to experimental measurements. The effects of the irradiation and fuel fabrication conditions (i.e., fission rate, fuel grain size, and mechanical work induced deformation) on the bubble evolution and the resultant swelling are investigated. The current simulations provide a better understanding of intragranular gas bubble-induced swelling and a solid foundation for the future study of the nucleation and growth of intergranular gas bubbles and recrystallization in U-Mo fuel.

U-Mo alloys are promising fuels for future high-performance research reactors with low enriched uranium. Surface properties, such as surface energy, are important inputs for mesoscale simulations (e.g., phase field method) of fission gas bubble behaviors in irradiated nuclear fuels. The lack of surface energies of U-Mo alloys prevents an accurate modeling of the morphology of gas bubbles and gas bubble-induced fuel swelling. To this end, we study the surface properties of U-Mo system, including bcc Mo, α-U, γ-U, and γ U-Mo alloys. All surfaces up to a maximum Miller index of three and two are calculated for cubic Mo and γ-U and non-cubic α-U, respectively. The equilibrium crystal shapes of bcc Mo, α-U and γ-U are constructed using the calculated surface energies. The dominant surface orientations and the area fraction of each facet are determined from the constructed equilibrium crystal shape. The disordered γ U-Mo alloys are simulated using the Special Quasirandom Structure method. The (1 1 0) and (1 0 0) surface energies of γ U-7Mo and U-10Mo alloys are predicted to lie between those of γ-U and bcc Mo, following a linear combination of the two constituents’ surface energies. To better compare with future measurements of surface energies, the area fraction weighted surface energies of α-U, γ-U and γ U-7Mo and U-10Mo alloys are also predicted.

We have developed a mesoscale phase-field model for studying the effect of recrystallization on gas-bubble-driven swelling in irradiated U-Mo alloy fuel. The model can simulate the microstructural evolution of the intergranular gas bubbles on the grain boundaries as well as the recrystallization process. Our simulation results show that the intergranular gas-bubble-induced fuel swelling exhibits two stages: slow swelling kinetics before recrystallization and rapid swelling kinetics with recrystallization. We observe that the recrystallization can significantly expedite the formation and growth of gas bubbles at high fission densities. The reason is that the recrystallization process increases the nucleation probability of gas bubbles and reduces the diffusion time of fission gases from grain interior to grain boundaries by increasing the grain boundary area and decreasing the diffusion distance. The simulated gas bubble shape, size distribution, and density on the grain boundaries are consistent with experimental measurements. We investigate the effect of the recrystallization on the gas-bubble-driven fuel swelling in U-Mo through varying the initial grain size and grain aspect ratio. We conclude that the initial microstructure of fuel can be used to effectively control the recrystallization and therefore reduce the swelling in U-Mo fuel.

To evaluate the effectiveness of ZrN as a diffusion barrier against fission gases, we investigate the incorporation and migration of fission gas atoms, with a focus on Xe, in ZrN by first-principles calculations. The formations of point defects in ZrN, including vacancies, interstitials, divacancies, Frenkel pairs, and Schottky defects, are first studied. Among all the defects, the Schottky defect with two vacancies as first nearest neighbor is predicted to be the most favorable incorporation site for fission gas Xe in ZrN. The migration of Xe gas atom in ZrN is investigated through two diffusion mechanisms, i.e., interstitial and vacancy-assisted diffusions. The migration barrier of Xe gas atom through the intrinsic interstitials in ZrN is considerably lower than that through vacancies. Therefore, at low temperatures fission gas Xe atoms diffuse mainly through interstitials in single crystal ZrN, whereas at high temperatures Xe may diffuse in ZrN assisted by vacancies.

A mesoscale model is developed by integrating the rate theory and phase-field models and is used to study the fission-induced recrystallization in U-7Mo alloy. The rate theory model is used to predict the dislocation density and the recrystallization nuclei density due to irradiation. The predicted fission rate and temperature dependences of the dislocation density are in good agreement with experimental measurements. This information is used as input for the multiphase phase-field model to investigate the fission-induced recrystallization kinetics. The simulated recrystallization volume fraction and bubble-induced swelling agree well with experimental data. The effects of the fission rate, initial grain size, and grain morphology on the recrystallization kinetics are discussed based on an analysis of recrystallization growth rate using the modified Avrami equation. We conclude that the initial microstructure of the U-Mo fuels, especially the grain size, can be used to effectively control the rate of fission-induced recrystallization and therefore swelling.

Atomistic simulation results of the (γU, βZr) solid solution behavior are discussed, including the behavior of the lattice parameter and coefficient of thermal expansion as a function of concentration and temperature. Output from these calculations is used to study the surface structure of U–Zr for different crystallographic orientations, determining the respective concentration profiles, surface energy, and segregation behavior. The segregation of Zr to the surface and overall composition of the near-surface region is studied as a function of concentration and temperature.