Anomalous behavior of nonequilibrium excitations in U O 2
Ultrafast optical pump-probe studies of uranium dioxide (UO 2 ) under pressure were performed in order to better understand the material's response to ionizing radiation. Photoexcitation generates oscillations in the time-resolved reflectivity at two distinct GHz-scale frequencies. The higher-frequency mode is attributed to a coherent longitudinal acoustic mode. The lower-frequency mode does not correspond to any known excitation under equilibrium conditions. The frequency and lifetime of the low-frequency mode are studied as a function of pressure. Abrupt changes in the pressure-dependent slopes of these attributes are observed at ~10 GPa, which correlates with an electronic transition in UO 2 . Variation of probe wavelength reveals that the low- k dispersion of the low-frequency mode does not fit into either an optical or acoustic framework. Rather, we propose that this mode is related to the dynamical magnetic structure of UO 2 . As a result, the implications of these results help account for the anomalously small volume of damage known to be caused by ionizing radiation in UO 2 ; we propose that the existence of the low-frequency mode enhances the material's transient thermal conductivity, while its long lifetime lengthens the timescale over which energy is dissipated. Both mechanisms enhance damage recovery.