The information contained in time-resolved PEI experiments was studied. A nonperturbative quantum mechanical theory was applied to compute the time-resolved differential cross section for a polyatomic molecule. Focus was on the case of an ultrafast radiationless transition. It was shown that the energy-resolved ionization asymmetry parameters, derived from PEI, serve to map the electronic population dynamics, effectively filtering out the vibrational dynamics with which the electronic modes are strongly coupled.
ASJC Scopus subject areas
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry