Vibrational predissociation from different asymmetric rotor levels: full dimensional quantum dynamics for ArI2 with total angular momentum J = 10

Full dimensional wavepacket calculations were carried out on ArI2 vibrational predissociation with total angular momentum J = 10. For five different values of initial I2 excitation, we consider the 21 lowest energy levels, corresponding roughly to the 2J + 1 asymmetric rotor levels superimposed on the zero-point motion of the Van der Waals degrees of freedom. In spite of the increased number of available states as J increases, fragmentation occurs via a sparse limit intramolecular vibrational energy redistribution mechanism involving passage through a few intermediate dark states. In addition, averaging over the rotor states does not negate or even decrease vibrational specificity.