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The elementary steps of the photodissociation and recombination reactions of iodine molecules enclosed in cages and channels of zeolite crystals: A femtosecond time-resolved study of the geometry effect Ion imaging is employed to analyze the fragments from timed Coulomb explosion studies of femtosecond ͑fs͒ molecular dynamics. The technique provides high detection efficiency and direct recording of the two-dimensional velocity of all ionized fragments. We illustrate the approach by studying photodissociation of iodine initiated by a weak femtosecond pump pulse and probed by an intense, delayed femtosecond pulse. The ion images, recorded as a function of the pump-probe delay, reveal the evolution of the internuclear separation of the dissociating I 2 molecule. The experimental results are in good agreement with quantum mechanical wave packet simulations. We discuss the perspectives for extending the studies to photochemical reactions of small polyatomic molecules.

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