One-photon ionization by a pulsed VUV laser has been employed to probe infrared multiphoton excitation and dissociation (IR-MPE/D) dynamics in real time, in situ, and collision free during excitation by a CO2− laser pulse. In this first experiment acetic anhydride has been used as the parent molecule to demonstrate the feasibility and to study properties of the method. Using the 118.4 nm radiation from a VUV laser as source for photoionization, ions have been observed mass selectively with time resolution in the nanosecond range, determined by the laser pulse duration. By following production and decay rates of ions, the time dependence of the excitation and decay of parent molecules, and the evolution of neutral intermediates in primary and sequential steps could be observed, from which detailed information on excitation and dissociation pathways was deduced.
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Feldmann et al. (1983) studied this question.
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