Coherent control and time-dependent density functional theory: towards creation of wave packets by ultrashort laser pulses

Explicitly time-dependent density functional theory (TDDFT) is a formally exact theory, which can treat very large systems. However, in practice it is used almost exclusively in the adiabatic approximation and with standard ground state functionals. Therefore, if combined with coherent control theory, it is not clear which control tasks can be achieved reliably, and how this depends on the functionals. In this paper, we continue earlier work in order to establish rules that answer these questions. Specifically, we look at the creation of wave packets by ultrashort laser pulses that contain several excited states. We find that (i) adiabatic TDDFT only works if the system is not driven too far from the ground state, (ii) the permanent dipole moments involved should not differ too much, and (iii) these results are independent of the functional used. Additionally, we find an artifact that produces fluence-dependent excitation energies.