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.