The multiphoton photoionization mechanisms in ultracold nitric oxide have been investigated via one- and two-color laser excitation in a supersonic expansion. Photoelectron spectroscopy is used to identify the roles of direct ionization, autoionization, and Rydberg-valence mixing for multiphoton ionization via several Rydberg states (A, E, H, F, N) of nitric oxide. Accidental double resonance with mixed Rydberg-valence states in the third-photon region of a nominally (2+2) multiphoton ionization is shown to yield non-Franck–Condon photoelectron distributions. However, non-Franck–Condon peaks can also appear when the third-photon region is either eliminated by frequency doubling or uniquely determined by using two-color excitation.
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Miller et al. (1986) studied this question.
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