Effects of multi orbital contributions in the angular-dependent ionization of molecules in intense few-cycle laser pulses

We outline the details of our new method to calculate angular-dependent ionization probabilities based on electronic structure theory for diatomic and larger systems. To demonstrate its abilities, we compare our calculations to measured ionization probabilities of the four molecules D₂, N₂, O₂ and CO in the strong-field regime. The calculated angular distributions yield better agreement with the experimental data than those obtained from the widely used MO-ADK theory. For CO the measured angular distributions of ionic fragments indicate contributions to the ionization from both the HOMO and the HOMO-1 orbital, an effect that is addressed by the theory.