We present a study of nonsequential double-recombination (NSDR) high-harmonic generation (HHG) in a molecularlike system. We have calculated the HHG spectrum for a wide range of internuclear distances, and using a Coulomb-corrected three-step model we are able to analyze and predict the observed NSDR HHG cutoffs precisely for all internuclear distances. It is shown through this Coulomb-corrected three-step (CC-TSM) model that there is an intrinsic dependence on the location of the nuclei in the NSDR HHG process not seen in one-electron HHG. This dependence originates from the strong electron correlation in the NSDR HHG process, and it modifies the classically allowed return energies which in return changes the cutoffs observed in the HHG spectra. It is observed that the CC-TSM correctly predicts cutoffs at all internuclear distances with differences of more than six harmonics being observed between the CC-TSM and the normal three-step model for the laser parameters used. We also observe that the NSDR HHG process changes for internuclear distances of $R\gtrsim 8–9$ a.u., which is proposed to stem from a change in the charge-transfer dynamics within the molecule. For large internuclear distances of $R\gtrsim 13$ a.u., we observe a clear signature of the point of emission for the first electron emitted in the NSDR HHG signal and we also see signs of molecular exchange paths contributing to the HHG spectrum for these internuclear distances.

• Received 8 December 2016
• Revised 9 May 2017

DOI:https://doi.org/10.1103/PhysRevA.96.013401