Multi-Plateau Molecular High Harmonic Generation Frome Multi-Functional Group Recombination

Abstract Permanent dipole moments induced high-order harmonic generation (HHG) signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources. Previous studies on this topic have mainly focused on diatomic molecules such as CO and HeH. Based on this scheme, significant HHG signals in the direction perpendicular to the molecular axis can be observed in both the high-energy and low-energy regions. However, we found that the high-order harmonics induced by the permanent dipole moments of polyatomic complex molecules involve more intricate physical processes. Using time-dependent density functional theory, we simulated the dynamics of HHG from NH 2 COOH and NH 2 COSH interacting with linearly polarized lasers. We found that the harmonic signals in the direction perpendicular to the N-C bond were significantly enhanced in the high-energy photon region. Our analysis indicates that this is due to the complex molecular configuration of NH 2 COOH and NH 2 COSH: while the NH 2 group has C 2 v symmetry, both COOH and COSH groups lack this symmetry. This structural characteristic results in permanent dipole moments being felt only when electrons return to either COSH or COOH groups, but not to NH 2 group. Additionally, our results reveal a multi-plateau structure in HHG signal along laser polarization direction, a phenomenon arising from multi-electron and multi-orbital effects during interaction between complex molecule and strong laser field.