Solid state–like high harmonic generation from cluster molecules with rotational periodicities

High harmonic generation (HHG) from solid-state crystals in strong laser fields has been understood by the band structure of the solids, which is based on the periodic boundary condition (PBC) due to translational invariance. For the systems with PBC due to rotational invariance, an analogous Bloch theorem can be applied. Considering a ring-type cluster of cyclo[18]carbon as an example, we develop a quasi-band model and predict the solid state–like HHG in this system. Under the irradiation of linearly polarized laser field, cyclo[18]carbon exhibits solid state–like HHG originated from intraband oscillations and interband transitions, which, in turn, is promising to optically detect the symmetry and geometry of molecular or material structures. Our results based on the Liouville–von Neumann equations are well reproduced by the time-dependent density functional theory calculations and are foundational in providing a connection linking the HHG physics of gases and solids.