High-order harmonic generation by aligned homonuclear diatomic cations

We introduce the theory of high-order harmonic generation by aligned homonuclear diatomic cations using a strong-field approximation. The target cation is represented as a system which consists of two atomic (ionic) centres and one active electron, while the driving field is either a monochromatic or bichromatic field. For a linearly polarised driving field, we investigate the differences between the harmonic spectra obtained with a neutral molecule and the corresponding molecular cation. Due to the larger ionisation potential, the molecular cations can withstand much higher laser-field intensity than the corresponding neutral molecule before the saturation effects become significant. This allows one to produce high-order harmonics with energy in the water-window interval or beyond. Also, the harmonic spectrum provides information about the structure of the highest-occupied molecular orbital. In order to obtain elliptically polarised harmonics, we suggest that an orthogonally polarised two-colour field is employed as a driving field. In this case, we analyse the harmonic ellipticity as a function of the relative orientation of the cation in the laser field. We show that the regions with large harmonic ellipticity in the harmonic energy-orientation angle plane are the broadest for cations whose molecular orbital does not have a nodal plane. Finally, we show that the molecular cations exposed to an orthogonally polarised two-colour field represent an excellent setup for the production of elliptically polarised attosecond pulses with a duration shorter than 100 as. We introduce the theory of high-order harmonic generation by homonuclear diatomic cations. The elliptically polarised harmonics can be produced using the orthogonal two-colour field and the cations whose molecular orbital does not have nodal planes.