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Quantum dynamical simulations of ultrafast processes of F 2  in an Ar matrix induced by a pump laser pulse show that photoexcitation (i) is followed by (ii) a stretch of the dissociative bond, (iii) collision with, vibrational excitations of, and possible exit through the nearest neighbour atoms of the surrounding cage, and (iv) finally, subsequent rescattering of the dissociated atoms causing vibrations of additional matrix atoms. If the laser pulse ended before the onset of process (iii), the initial steps (i) and (ii) are similar to photodissociations in the gas phase and are, therefore, well described in terms of the wavepacket dynamics of the diatomic molecule in reduced dimensionality. For specific symmetry constraints, the initial processes (i), (ii), and (iii) may be described in terms of just 1- and 2- or 3-dimensional wavepacket dynamics, respectively. At the end of the laser pulse, this low-dimensional wavepacket may serve to prepare the high-dimensional one for the subsequent laser-free dynamics of the total system.

Initial Processes of Laser Induced Diatomic Molecular Photodissociation in Matrices: Quantum Simulations for F 2 in Ar in Reduced Dimensionality