Short-time effects in light absorption

M. Simhony

Joachım Herrmann, J. Wienecke, B. Wilhelmi

Y. B. Band

We describe the absorption characteristics of polarized light pulses of short temporal duration in media with a ground state absorption cross section and large excited state absorption cross section. The effects of rotational diffusion, pulse depletion, finite pulse propagation time, and transition dipole moment orientation are properly treated. Significant enhancement of the reverse saturation due to excited state absorption results when the ground and excited state absorption dipole moments are parallel.

E. U. Condon

W. Vogel, D.‐G. Welsch, B. Wilhelmi

The dependence of the electronic absorption spectrum of a dye molecule on the time of delay between the excitation of the molecule by a pump-laser pulse and the probing of the absorption by a test-laser pulse is studied. The effect of dephasing of the molecular transition arising from the interaction with dissipative systems is described by a stochastic modulation of the electronic transition frequency. It is shown that in the case when the two laser pulses are short compared with the correlation time of the frequency modulation and when the spectral linewidth of the pump-laser light is smaller than the bandwidth of the equilibrium absorption spectrum, hole burning appears although the molecules have equal mean transition frequencies. This effect arises from non-Markovian correlations between the dephasings of the molecule during the actions of the pump- and the test-laser pulse. With increasing delay time the holes are smoothed out and disappear when the delay time exceeds the correlation time. Such effects were found in recent femtosecond absorption experiments by Shank et al. [in Ultrafast Phenomena V, dited by G. R. Fleming and A. E. Siegman (Springer, Berlin, 1986), p. 179].