Dynamical interference structures in fully coupled bound-bound state quantum wave-packet dynamics

The quantum wave-packet dynamics in a bound-bound state system at intermediate coupling strength, the A and b states in the Rb₂ molecule coupled by spin-orbit interaction, was studied by ultrafast pump-probe molecular beam spectrocopy and quantum dynamical calculations. It was shown that even at elevated molecular temperatures the experimentally observed traces are characterized by dynamical interference structures of mesobatic, i.e., diabatic-adiabatic hybrid, kind. Two types of mesobatic motion were discerned: bistable, which occurs in both bound-unbound and bound-bound systems, and astable, which is particular to bound-bound systems at intermediate coupling strength. Contrary to previous expectations, the signatures of the quantum interference structures in pump-probe delay traces were found to be robust toward averaging over initial quantum states. It was shown that the spectral variations observed while tuning the pump pulse wavelength is a quantum matter-wave relative of the fringes observed in a pulsed optical Michelson interferometer.