Elliptic Dichroism in the Above-Threshold Ionization of Molecules Induced by a Strong Laser Field

J Phys Chem A. 2023 Oct 5;127(39):8209-8219. doi: 10.1021/acs.jpca.3c03965. Epub 2023 Sep 21.

Abstract

Using a strong-field-approximation theory, we investigate the high-order above-threshold ionization of diatomic molecules exposed to the monochromatic and bichromatic elliptically polarized fields. We devote particular attention to the difference between the photoelectron momentum distributions obtained with fields with opposite helicity. This difference is quantified using the elliptic-dichroism parameter, which represents the normalized difference between the differential ionization rates calculated with driving fields with opposite helicity. We find that this parameter strongly depends on the molecular orientation with respect to the laser field. In addition, this dependence is different for molecules with different types of highest-occupied molecular orbital. In other words, we show that the molecular structure is imprinted onto the elliptic-dichroism parameter for both monochromatic and bichromatic driving fields. This is explained by analyzing the interferences between various partial contributions to the differential ionization rate. In this way, elliptic dichroism also serves as a tool to analyze the electron dynamics. Finally, for heteronuclear diatomic molecules, we show that the elliptic dichroism is different from zero even for the direct electrons, i.e., the electrons that after liberation go directly to the detector. In this case, the dependence on the molecular orientation is far more pronounced for a bichromatic driving field.