A Numerical Study of Pulse-Shape Control of Non-Adiabatic Electron Excitation in the Strong-Field Regime

The electron optical response of several molecular monocations to short strong-field laser pulses was studied using time-dependent Hartree-Fock theory. In addition to the carrier frequency and maximum amplitude (up to 3.75 x 10$^{13}$ W/cm$^{2})$, the short pulses were characterized by pulse shape parameters: the amplitude profile (trapezoidal and gaussian) and the carrier phase shift. The electron response was traced by the evolution of the excited states occupation numbers and by the instantaneous dipole moment of the molecule. In the molecular monocations studied, butadiene, naphthalene, and anthracene, we observed significant modifications in the dipole moment response and in the corresponding excited state spectra, controlled by intensity, frequency, phase, and shape of the laser pulse.