Abstract

Publisher Summary Doubly excited states play a major role in the reaction dynamics of diatomic molecules as these states directly couple the different continua of dissociation and ionization. Electronic autoionization and neutral dissociation are therefore competing processes, but information from both channels may be used to characterize the doubly excited molecular states. Application of femtosecond (fs) laser pulses considerably facilitates the interpretation of fragmentation processes because the time duration of a laser pulse is much shorter than the fragmentation separation time. Femtosecond pulses are generated in a home-built colliding-pulse-mode-locked ring dye laser (CPM) with four intracavity prisms to adjust for the group. This chapter illustrates the use of fs-laser in combination with ion- and electron spectroscopy to clarify the ionization and fragmentation pathways of molecules excited by multiphoton processes.

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