Phonons and electron-phonon interactions in rare-gas crystals at high pressures

Abstract

The lattice dynamics of compressed rare-gas crystals is theoretically investigated within the ab initio approach in the framework of the Tolpygo model, which explicitly allows for the deformation of electron shells. The deformation of the electron shells is associated with the retardation of the electron response and treated as a nonadiabaticity (the electron-phonon interaction). This approach and the ab initio short-range repulsive potentials are used to construct the dynamic matrix, which makes it possible to calculate the phonon frequencies and the electron-phonon interaction of crystals in the series Ne-Xe at any point of the Brillouin zone. The contributions of the long-range Coulomb and van der Waals forces to the dynamic matrix are the structure sums that depend only on the lattice type. The structure sums for the face-centered cubic lattice are calculated using the Ewald and Emersleben methods, as well as the direct summation over the vectors of the face-centered cubic lattice. The use of 20 spheres in the last case provides an accuracy of no less than four significant figures. An analysis of the role played by the phonon-electron interaction at five points of high symmetry in the Brillouin zone (X, L, U, K, W) at high pressures demonstrates that not only the longitudinal phonon modes (at the points X and L) but also the transverse phonon modes (at the points U, K, and W) are softened. The inclusion of the electron-phonon interaction at the point X improves agreement between the theoretical and experimental phonon frequencies for the argon crystal.