Optimal pulse for orbital reconstruction from ionization maps in aligned molecules

We perform ab initio calculations on the total ionization probability of diatomic molecules in strong laser fields as a function of alignment angle, the angle between the laser polarization and the molecular axis, with the goal of investigating whether these ionization maps can be used to determine the orbital symmetry of the initial state. We find that the ionization rate for each alignment angle is highly dependent on the pulse intensity and duration and, because of this dependence, the orbital symmetry can only be determined with the appropriate pulse parameters. The pulse length and intensity need to be chosen in such a way as to avoid excessive ionization, or significant population of other bound states. We also observe that the internuclear separation of the molecule strongly affects the mapping of the orbital symmetries.