Nonadiabatic generation of coherent phonons

Abstract

The time-dependent density functional theory (TDDFT) is the leading computationally feasible theory to treat excitations by strong electromagnetic fields. Here the theory is applied to coherent optical phonon generation produced by intense laser pulses. We examine the process in the crystalline semimetal antimony (Sb), where nonadiabatic coupling is very important. This material is of particular interest because it exhibits strong phonon coupling and optical phonons of different symmetries can be observed. The TDDFT is able to account for a number of qualitative features of the observed coherent phonons, despite its unsatisfactory performance on reproducing the observed dielectric functions of Sb. A simple dielectric model for nonadiabatic coherent phonon generation is also examined and compared with the TDDFT calculations. © 2012 American Institute of Physics.