Effects of electron structure and multielectron dynamical response on strong-field multiphoton ionization of diatomic molecules with arbitrary orientation: An all-electron time-dependent density-functional-theory approach

Abstract

We present a time-dependent density-functional-theory approach for the ab initio study of the effect of correlated multielectron responses on the multiphoton ionization (MPI) of diatomic molecules N2, O2, and F2 in intense short laser pulse fields with arbitrary molecular orientation. We show that the contributions of inner molecular orbitals to the total MPI probability can be significant or even dominant over the highest-occupied molecular orbital, depending on detailed electronic structure and symmetry, laser field intensity, and orientation angle.