Abstract

The multiphoton ionization spectrum of nitric oxide cooled by a supersonic expansion has been recorded in the region 400–490 nm. The cooling of rotational degrees of freedom has allowed analysis of the two- and three-photon resonances observed in this region, and it is found that the simple extension of one-photon intensity relationships to the three-photon spectrum is unwarranted. The relative intensities of the two- and three-photon resonances support the notion that a kinetic rate equation description provides a basic framework for the interpretation of multiphoton ionization spectra initiated by a pulsed, multimode dye laser. The role of predissociation in the observed spectra is discussed.

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