A numerical study on vibronic and vibrational dynamics generated by chirped laser pulses in the presence of relaxation processes

Detailed mechanisms of creation and destruction of coherence and population generated by the chirped pulses in the presence of the relaxation processes are numerically investigated. It is found that, during the intra-pulse pump–dump process of the negatively chirped pulse laser excitation, the vibronic coherence is sequentially created between the electronically excited and ground states. In this case, the pure dephasing process affects the time-ordered creation process of the population of each vibrational state in the electronically excited state.