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Journal of the Optical Society of America B

Optical Stark effect in molecules probed by 10-fs optical pulses

R. L. Fork, C. H. Brito Cruz, Charles V. Shank

Published Jan 1, 1987• 0 citations
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Abstract

In earlier work we used 10-fs optical pulses to probe the dynamics of spectral hole burning in dye molecules excited within their absorption bands by 60-fs pump pulses.1 In this work we use probe pulses of 10-fs duration to examine the dynamics of dye molecules excited below their absorption resonances. The optical Stark effect is found to play an important role in the induced dynamics.

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•May 1, 1990•0 citations
In earlier work we used 10-fs optical pulses to probe the dynamics of spectral hole burning in dye molecules excited within their absorption bands by 60-fs pump pulses.1 In this work we use probe pulses of 10-fs duration to examine the dynamics of dye molecules excited below their absorption resonances. The optical Stark effect is found to play an important role in the induced dynamics.
An external field applied to dye doped polymers which have inhomogeneous dispersion in their absorption spectra causes a shift in the absorption of the dye molecules. This, in turn, changes the line shapes of persistent spectral holes1). The Stark effect has been applied to optical storage2) and optical computing3). It has been also used as a powerful tool for investigating such physical profiles of materials as the difference between the effective molecular electric dipole moments in the host matrix in the ground and excited states which is related to hole burning4),5).
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].
The theory of the optical Stark effect is developed for quantum-size structures. The effect is due to the interaction of the electron system with intense light, whose frequency, (omega) , is in resonance between two subbands in the conduction band. The probe light of the frequency (Omega) falls in resonance with the adjacent transition between the ground state and the state with an electron-hole pair. In the quasi-steady-state mode, the singularities in the interband (Omega) -light absorption spectra are related to the critical points of the bands, rearranged by the (omega) - light. The shape of the higher conduction band can be evaluated from the spectral positions of the singularities. In the case of two-photon interband transitions, a sharp dependence of the absorption on the light intensity is predicted. In the non-steady-state mode, the probe beam consists of two femtosecond (Omega) -light pulses following each other with the delay time, (tau) d. The dependence of energy, absorbed from the second pulse, on the (tau) d value is calculated. Under the (omega) -pumping, one of the two phenomena should be observed, depending on the type of band structure, namely, the decay of the induced polarization with the characteristic time approximately 1/(omega) R or oscillations with the frequency approximately (omega) R, where (omega) R is the Rabi frequency. The principal effect, controlling the decay of the Rabi oscillations, is the spreading of the packet of states generated by the (Omega) -light pulse.
A model calculation is presented that describes the features of spectral-hole burning measurements performed under conditions of femtosecond transient excitation and probing. Pump-induced changes in the spectrum of probe transmittance arise not only from changes in level population (hole burning), but also from the presence of pump polarization during the probe, and from perturbations of the decay of the probe polarization. These latter effects give rise to oscillating differential transmittance spectra when the (shorter) probe pulse arrives prior to the peak of the pump noise. Only when the probe pulse follows the bulk of the pump pulse does the level population effect dominate the spectrum, so that one can observe dynamic hole-burning effects without distortion.>
We show that in order to describe completely the coherent coupling between the pump and probe pulses in a pump– probe measurement of transient absorption, the influence of induced phase gratings must be included. The importance of phase gratings is demonstrated experimentally for the case of a bleachable dye and analyzed in terms of transient four-wave mixing. These results are relevant to the interpretation of pump–probe measurements on all time scales performed with pulses from a single laser, particularly when the pulse duration is comparable with the material response time.