Dynamical theory of spectroscopy with femtosecond pulse excitation (Q1392648)

The development of the femtosecond pulsed laser technique and its application in chemistry enable us to trace and measure a chemical reaction in real-time possibly. One of the most interesting examples is the direct dissociation with femtosecond pulse excitation. The reaction of this type can be expressed as \(M+h\nu\to M'+M''\). After a molecule is excited to a dissociative continuum by a femtosecond pulse, it propagates on the excited state while it falls apart into some new fragments \(M'\) and \(M''\). This process usually lasts about tens of femtoseconds. Because the fullwidth half-maximum of the pulse is much shorter than the molecular vibrational period, the emitted signal thus observed is expected to be very sensitive to the events taking place in the dissociation process. The dynamical theory of spectroscopy with femtosecond pulse excitation is applied to a direct dissociation process. In the ultrashort pulse case, the fluorescence-like emission peak occurs in Raman scattering as the incident frequency is tuned near resonance. All properties of the spectroscopy can be explained by the correlation function.