Imprints of multielectron polarization effects in odd-even harmonic generation from CO molecules

Abstract

Dynamic core-electron polarization (DCeP) is a correction to the single-active electron (SAE) approximation by considering a response of the core electrons to the time-dependent laser field. Despite being initially construed as a perturbative correction, in some cases especially atoms and molecules with large polarizabilities, DCeP can qualitatively alter predictions produced by the bare SAE theory. In this study, we unambiguously demonstrate the nonperturbative role of DCeP in the resolved odd-even high-order harmonic generation (HHG) of the CO molecule. In particular, we find that the even-to-odd ratio, i.e., the ratio between the harmonic intensities of even order and average of the two adjacent odd orders, changes by as much as one order of magnitude when DCeP is included, making the theoretically predicted values remarkably consistent with the experimental ones. This strong manifestation allows us to verify the DCeP role in HHG by experimental data. Furthermore, our analysis of the harmonic time profile shows that this agreement is not an artifact of the numerical method but reflects relevant physics, establishing that DCeP must be incorporated into the standard framework for strong-field physics.