Role of the electronic structure and multielectron responses in ionization mechanisms of diatomic molecules in intense short-pulse lasers: An all-electron ab initio study

The importance of the electronic structure and multielectron responses in the ionization mechanism of diatomic molecules in intense short-pulse lasers was analyzed using an all-electron ab initio study. The contributions of inner valence electrons to the molecular multiphoton ionization (MPI) of diatomic molecules in strong laser fields were also investigated. The inner valence electron ionization was found to be related to the orbital orientation and the enhanced dipole coupling between molecular orbitals at high laser intensities. The results show that the multielectron responses of a molecule enhance or supress the ionization of individual electrons.