High-order above-threshold ionisation of diatomic molecules by few-cycle bicircular and orthogonally polarised...

Improved molecular strong-field approximation theory is used to calculate the ionisation probability for the high-order above-threshold ionisation process induced by a few-cycle pulse with two carrier frequencies and one envelope. The asymmetry in the photoelectron momentum distribution is due to the ultrashort nature of the driving pulse and due to the relative orientation of the molecule with respect to the laser field. We introduce the generalised asymmetry parameter, which can be used to quantitatively measure the asymmetry between the photoelectron spectra along arbitrarily many selected directions. We investigate the difference between the asymmetry parameters calculated for atomic and molecular targets and show that the contributions to the asymmetry strongly depend on the type of the employed driving pulse. For the driving pulse with components that are linearly polarised with mutually orthogonal polarisations, we find that the main source of the asymmetry, especially in the high-energy part of the spectrum, is the ultrashort nature of the pulse. The relative orientation of the molecule with respect to the laser pulse only affects the low- and medium-energy parts of the spectrum. On the other hand, for the driving pulse with circularly polarised counterrotating components, the asymmetry introduced by molecular orientation is more pronounced. We also analyse the influence of the characteristics of molecular orbitals on the asymmetries using the examples of N₂ and O₂ molecules.