Ultrafast non-adiabatic dynamics of systems with multiple surface crossings: a test of the Meyer–Miller Hamiltonian with semiclassical initial value representation methods

Three three-state models have been studied to test the capabilities of the Meyer–Miller Hamiltonian studying non-adiabatic photodissociation dynamics. within the framework of the semiclassical initial value representation (SC-IVR). The absorption spectra and the evolution of the electronic populations were calculated using the SC-IVR methodology, and they both show excellent agreement with accurate quantum results. A linearized version (LSC-IVR) was also tested, and it describes the dynamics well for short times but becomes less accurate at longer time.