We have measured the room-temperature phonon spectrum of Mo-stabilized γ-U. The dispersion curves show unusual softening near the H point, q = [1/2, 1/2, 1/2], which may derive from the metastability of the γ-U phase or from strong electron-phonon coupling. Near the zone center, the dispersion curves agree well with theory, though significant differences are observed away from the zone center. The experimental phonon density of states is shifted to higher energy compared to theory and high-temperature neutron scattering. The elastic constants of γ-UMo are similar to those of body-centered cubic elemental metals.

Recent X-ray measurements suggest a degree of valence fluctuation in plutonium and uranium intermetallics. We are applying a novel scheme, in conjunction with density functional theory, to predict 5f configuration fractions of states with valence fluctuations for the early actinide metals. For this purpose we perform constrained integer f-occupation calculations for the α phases of uranium, neptunium, and plutonium metals. For plutonium we also investigate the δ phase. The model predicts uranium and neptunium to be dominated by the f3 and f4 configurations, respectively, with only minor contributions from other configurations. For plutonium (both α and δ phase) the scenario is dramatically different. Here, the calculations predict a relatively even distribution between three valence configurations. The δ phase has a greater configuration fraction of f6 compared to that of the α phase. The theory is consistent with the interpretations of modern X-ray experiments and we present resonant X-ray emission spectroscopy results for α-uranium.

We report a comprehensive structural and valence study of the intermediate valent materials YbNiGa4 and YbNiIn4 under pressures up to 60 GPa. YbNiGa4 undergoes a smooth volume contraction and shows steady increase in Yb valence with pressure, though the Yb valence reaches saturation around 25 GPa. In YbNiIn4, a change in pressure dependence of the volume and a peak in Yb valence suggest that a pressure-induced electronic topological transition occurs around 10-14 GPa. In the pressure region where YbNiIn4 and YbNiGa4 possess similar Yb-Yb spacings, the Yb valence reveals a precipitous drop. This drop is not captured by density functional theory calculations and implies that both the lattice degrees of freedom and the chemical environment play an important role in establishing the valence of Yb.