Spectral intensity and phase changes of short laser pulses by two-photon absorption

We calculated third order non-linear polarization to estimate the two-photon absorption of non-interacting two-level molecules in the transmission-type degenerate pump–probe geometry. The spectral intensity and the phase changes of the laser pulses when passing through a thin dielectric slab composed of the molecules were considered. We also investigated the effect of the decay rate of the molecules and the chirp of the pulses on their spectral intensity and phase changes.