Perturbative treatments of pump–probe laser‐molecule ...

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Title Perturbative treatments of pump–probe laser‐molecule interactions with applications to azulene and trimethylazulene
Author(s) P. Tran, W. J. Meath, Brian D. Wagner, R. P. Steer
Journal Journal of Chemical Physics
Date 1994
Volume 100
Issue 6
Start page 4165
End page 4170
Abstract Semianalytic perturbative approaches for investigating the spectroscopy, and the underlying dynamics, associated with fast time-resolved, two-photon, two-color, pump-probe, low intensity laser-molecule interactions are developed and discussed. In particular the perturbation theory is developed with emphasis on molecular models associated with pump-probe experiments on the S-0-->S-1-->S-2 two-photon transitions in azulene and trimethylazulene. The experiments are discussed and the theory is used to determine the lifetimes of the intermediate S-1 states by analyzing the experimental two-photon fluorescence signals from the S-2 states as a function of the time-delay between the pump and probe lasers. The advantages of using this approach relative to the traditional methods for determining the lifetime of the S-1 states are discussed. The dependence of the two-photon fluorescence signals on the angle between the polarization vectors of the pump and probe lasers, for fixed time delay between the lasers, is also considered briefly.
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