Time-resolved dynamics of odd and even harmonic emission from oriented asymmetric molecules

We study the time-resolved dynamics of high-order harmonic generation (HHG) from oriented asymmetric molecules in intense laser fields theoretically. Previous studies have shown that the odd-even HHG spectra of asymmetric molecules don't show the striking two-center-interference-induced minimum, as the symmetric molecules do, due to the symmetry breaking. Surprisingly, with considering only the short-trajectory contribution, an apparent groove with small amplitudes is observed in the HHG time-frequency distribution, which implies that the harmonic emission is strongly suppressed in a specific time-frequency region. The position of this groove is sensitive to the molecular parameters and the orientation. Our analyses on this origin of the groove reveal different time-frequency properties of odd versus even signals, where the interplay of intramolecular interference and the permanent-dipole effect plays an important role. We show that the even-odd ratio often used in high-harmonic spectroscopy can be influenced significantly by the interference effect.