Non-adiabatic quantum molecular dynamics: Generalized formalism including laser fields

Abstract

A generalized formalism of the so-called non-adiabatic quantum molecular dynamics is presented, which applies for atomic many-body systems in external laser fields. The theory treats the nuclear dynamics and electronic transitions simultaneously in a mixed classical-quantum approach. Exact, self-consistent equations of motion are derived from the action principle by combining time-dependent density functional theory in basis expansion with classical molecular dynamics. Structure and properties of the resulting equations of motion as well as the energy and momentum balance equations are discussed in detail. Future applications of the formalism are briefly outlined.