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High Phonon Scattering Rates Suppress Thermal Conductivity in Hyperstoichiometric Uranium Dioxide

Uranium dioxide (UO$_2$), one of the most important nuclear fuels, can accumulate excess oxygen atoms as interstitial defects, which significantly impacts thermal properties. In this study, thermal conductivities and inelastic neutron scattering measurements on UO$_2$ and UO$_{2+x}$ (x=0.3, 0.4, 0.8, 0.11) were performed at low temperatures (2-300 K). The thermal conductivity of UO$_{2+x}$ is significantly suppressed compared to UO$_2$ except near the Néel temperature TN= 30.8 K, where it is independent of x. Phonon measurements demonstrate that the heat capacities and phonon group velocities of UO$_2$ and UO$_{2+x}$ are similar and that the suppressed thermal conductivity in UO$_{2+x}$ results from high phonon scattering rates. These new insights advance our fundamental understanding of thermal transport properties in advanced nuclear fuels.