Chemical Physics Letters, Vol.336, No.3-4, 262-267, 2001
Manifestation of predissociation and vibrational relaxation in femtosecond pump-probe signals: a theoretical analysis
Classical molecular dynamics (MD) is used to study vibrational relaxation and predissociation processes in I-2 embedded in a rare-gas environment. It is shown that the simultaneous effect of the two mechanisms determines the deviation of experimental pump-probe signals from a single-exponential decay [Lienau and Zewail, J. Phys. Chem. 100 (1996) 18629].