Critical Examination of Explicitly Time-Dependent Density Functional Theory for Coherent Control of Dipole Switching.

We compare the performance of explicitly time-dependent density functional theory (DFT) with time-dependent configuration interaction (TDCI) to achieve the control task of a population inversion in LiCN. We assume that if a given pulse achieves the control task when used in TDCI, then there should be a pulse with similar frequency and intensity that achieves the task in time-dependent DFT (TDDFT). The present investigation indicates that this is not the case, if standard functionals are used in the adiabatic approximation.