Abstract

The vacuum ultraviolet (VUV) radiation is generated in the strong-field-ionized CO molecules through ${2} + {1}$ resonance excitation with two-color femtosecond laser pulses. When scanning the relative delay between two pump pulses, the rotational-resolved VUV radiations show periodic oscillations lasting as long as 500 ps. Fourier analysis reveals that these oscillations correspond to rotational beat frequencies of the ${{A}^2}{{\Pi}_{i}}$ state of ${{\rm CO}^ +}$, which is the result of multi-channel interference during the resonant excitation process. High resolution of Fourier transform spectra up to ${0.067}\;{{\rm cm}^{- 1}}$ allows us to obtain the fine energy levels of the ${{A}^2}{{\Pi}_{i}}$ state. The theoretical calculation is in good agreement with the experimental observation. This work reveals the rotational coherence of the ionic excited state and shows the prospect of rotational coherence spectroscopy in measuring fine structures of molecular ions.

© 2021 Optical Society of America

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