Role of degenerate states on molecular excitation by intense laser pulses

A singlet diatomic molecule naturally carries a doubly degenerate ±Λ-state when the projection of the total electronic angular momentum onto the internuclear axis is nonzero. These doubly degenerate states contribute equally in conventional measurements and are thus treated the same in corresponding simulations. In this study, we demonstrate that in resonant excitation by intense laser pulses, the doubly degenerate ±Λ-state must be clearly identified. This is exemplified in the X 1 Σ → A 1 Π transition of CO molecules. This distinction becomes especially important in the case of circularly polarized radiation. We attribute this phenomenon to the interference of electron-rotational pathways in the strong-field coupled transition with the ±Λ-state of the excited Π state. This research sheds light on the fundamental aspects of intense laser-molecule interactions when extending conventional theories.