Abstract
The rotational structure of two-photon spectra of van der Waals complexes involving an open shell diatomic molecule is analyzed in terms of the spherical tensor components of the two-photon absorption operator of the uncomplexed diatom. The formalism is used to explain the rotational structure of several band systems of the NO–Ar complex correlating with Rydberg states of the bare NO molecule. All spectra recorded suggest an N–O bond distance typical for a Rydberg state. For the C 2Π state, the vibrationally averaged structure is T shaped. Within the effective experimental resolution no P-type doubling could be identified. For the bands correlating with the state E 2Σ, a significant deviation from the T-shaped structure is found. Once the rotational contour can be simulated, a complete analysis of the vibrational structure due to the intermolecular vibrations can be performed. For the Ar–NO E state, the bending and stretching frequencies suggest a close resemblance to the cationic complex Ar–NO+.
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