Phonon dispersion and low-energy anomaly in CaC6 from inelastic neutron and x-ray scattering experiments

We report measurements of phonon dispersion in CaC6 using inelastic x-ray and neutron scattering. We find good overall agreement, particularly in the 50 meV energy region, between experimental data and first-principles density-functional-theory calculations. However, on the longitudinal dispersion along the (111) axis of the rhombohedral representation, we find an unexpected anticrossing with an additional longitudinal mode, at about 11 meV. At a comparable energy, we observe also unexpected intensity on the in-plane direction. These results resolve the previous incorrect assignment of a longitudinal phonon mode to a transverse mode in the same energy range. By calculating the electron susceptibility from first principles we show that this longitudinal excitation is unlikely to be due to a plasmon and consequently can probably be due to defects or vacancies present in the sample. © 2010 The American Physical Society.