Control and analysis of single-determinant electron dynamics

Methods which use time-dependent orbitals for the description of quantum dynamics of electrons, like (multiconfiguration) time-dependent Hartree-Fock or time-dependent density-functional theory, produce an effectively time-dependent electronic structure. This effect is strongest if only a single determinant represents the system. Focusing on this case, we show how features of the time-dependent electronic structure show up in optimized laser pulses used for the coherent control task of a population inversion.