Phase structure of below-threshold harmonics in aligned molecules: a few-level model system

Abstract

We utilize few-level model systems to analyze the polarization and phase properties of below-threshold harmonics generated from aligned molecules. In a two-level system, we find that the phase of emitted harmonics undergoes a distinct change. For harmonics with photon energies below the transition energy between the dominant field-dressed states, the phase alternates by $\pi$ between successive odd harmonic orders. In contrast, the phase remains constant for harmonics above the transition energy. Exploiting this behavior, we construct a four-level model composed of two uncoupled two-level systems aligned along orthogonal directions. We demonstrate that with selected transition frequencies lower-order harmonics follow the polarization of the linearly polarized driving field while higher-order harmonics exhibit a mirrored polarization. The model predicts that aligned systems with orthogonal transition dipoles may show analogous phase and polarization features in the below-threshold regime.