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Title: Energy Frontier Research Center Center for Materials Science of Nuclear Fuels

Scientific Successes • The first phonon density of states (PDOS) measurements for UO2 to include anharmonicity were obtained using time-of-flight inelastic neutron scattering at the Spallation Neutron Source (SNS), and an innovative, experimental-based anharmonic smoothing technique has enabled quantitative benchmarking of ab initio PDOS simulations. • Direct comparison between anharmonicity-smoothed ab initio PDOS simulations for UO2 and experimental measurements has demonstrated the need for improved understanding of UO2 at the level of phonon dispersion, and, further, that advanced lattice dynamics simulations including finite temperatures approaches will be required for handling this strongly correlated nuclear fuel. • PDOS measurements performed on polycrystalline samples have identified the phonon branches and energy ranges most highly impacted by fission-product and hyper-stoichiometry lattice defects in UO2. These measurements have revealed the broad-spectrum impact of oxygen hyper-stoichiometry on thermal transport. The reduction in thermal conductivity caused by hyper-stoichiometry is many times stronger than that caused by substitutional fission-product impurities. • Laser-based thermo-reflectance measurements on UO2 samples irradiated with light (i.e. He) ions to introduce point defects have been coupled with MD simulations and lattice parameter measurements to determine the role of uranium and oxygen point defects in reducing thermal conductivity. • A rigorous perturbation theory treatmentmore » of phonon lifetimes in UO2 based on a 3D discretization of the Brillouin zone coupled with experimentally measured phonon dispersion has been implemented that produces improved predictions of the temperature dependent thermal conductivity. • Atom probe investigations of the influence of grain boundary structure on the segregation behavior of Kr in UO2 have shown that smaller amounts of Kr are present at low angle grain boundaries than at large angle grain boundaries due to the more dense dislocation arrays associated with large angle boundaries; this observation has potentially important ramifications for thermal transport in the high burn-up rim region of light water reactor fuel. • A variable charge interatomic potential has been developed that not only provides an accurate representation of the fluorite UO2 phase, it is further capable of describing continuous stoichiometry changes from UO2 to hyper-stoichiometric UO2+x, to U4O9 and U3O7, and possibly to orthorhombic U3O8. This is the first potential that features many-body effects in all possible interactions (U-U, U-O and O-O) combined with the variable charge. • A theoretical proof has been formulated showing that it is necessary to use the so-called model C phase field approach, consisting of Cahn-Hilliard and Allen-Cahn equations, to describe void evolution in irradiated materials. This work resolved a longstanding literature controversy regarding how to model voids at the mesoscale. • A novel cluster dynamics model has been developed for the nucleation of voids and loops in UO2 under irradiation. This model is important in understanding the defect state of UO2 after irradiation and, more importantly, reveals off-stoichiometric states of irradiated UO2 that are critical for understanding the impact of irradiation on thermal transport. Personnel Successes« less
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Resource Type:
Technical Report
Research Org:
Idaho National Laboratory (INL)
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Country of Publication:
United States
36 MATERIALS SCIENCE Materials Science; Nuclear Fuels