Time and angle resolved calculations in delayed photodissociation

Time-dependent calculations concerning delayed photodissociation of diatomic molecules are presented. The formalism is used to calculate the time-dependent anisotropy of the fragments resulting from photodissociation of H₂ via tunneling through the barrier of the i³Ý_g state. Only the rotational motion is treated time-dependently. The method presented is relatively simple and is non-perturbative in the treatment of the interaction with the photon field. Oscillations in the photofragment anisotropy and in the photofragment yield are predicted at all photon field strengths upon switching on the interaction. It is argued that these effects are amenable to experimental verification with present day pulsed laser systems.