We report what we believe to be the first observation of coherent transient absorption changes in glasses doped with quantum dots of CdS0.12Se0.88. These observations were made at room temperature with on-resonant laser pumping. We observe a transient bleaching on the high energy side of the pump center wavelength, and a transient absorption increase on the low energy side. The transient effects last for a time about equal to the pump pulse duration, 80 fsec, after which real carrier generation masks the effects. The results can be qualitatively explained by a spectral shift in the direction predicted by the optical Stark effect. This was a pump-probe experiment where the 622-nm pump center wavelength was on the long wavelength side of the lowest energy transition in the quantum dots but still well within the absorption band. The radii of the microcrystallites ranged from 20 to 40 Å, and T2 in similar samples was estimated to be 60 fsec or less. Although the laser pulsewidth is longer than the dephasing time in the sample, we were still able to see coherent effects.
Using laser pulses of duration comparable to semiconductor relaxation and dephasing times, the coherent phenomena common to two-level systems have been demonstrated in II-VI and III-V semiconductors. These light-matter interactions are characterized by electrons and holes in their initially excited states and/or a macroscopic polarization that persists after the excitation. A nonthermal carrier distribution was observed in bulk CdSe, demonstrating the extremely fast energy relaxation possible when carrier-LO-phonon scattering is included. Quantum-confined CdSe microcrystallites were then employed to limit the available decay avenues. The one and two-pair transitions were characterized, and using spectral hole-burning, energy relaxation was shown to be substantially slower than in bulk. Dipole dephasing remained very rapid. Persistent macroscopic polarization was demonstrated in semiconductors through pump and probe experiments conducted on time scales faster than the inverse linewidth of the exciton. In the first set of experiments, it was found that the exciton optical Stark shift deviates from that predicted by a steady-state theory. The shift is smaller than expected and lasts longer than the pump pulse. Both effects are explained by free evolution of the exciton's polarization. Transient exciton bleaching is observed and shown to be a result of adiabatic following. In a second study of coherent polarization, spectral oscillations at negative delay times were studied. Oscillations were measured in a wide variety of semiconductors, temporally preceding several different pump-probe phenomena. By comparison with a semiclassical theory, it was shown that spectral oscillations in the spectral region of the exciton are evidence of persistent exciton polarization. Oscillations in the band are due to four wave mixing of the pump and probe beams.
Phase relaxation of optical excitations in condensed matter can be studied by coherent four—wave—mixing experiments in the time domain without requiring assumptions on the spectral properties of the material. For inhomogeneously broadened transitions, three laser pulses at times t = 0, t = t21 and t = T with wave vectors k1, k2 and k3, respectively, generate a stimulated photon echo pulse, emitted time—delayed at t = T+t21 in the momentum—matching direction according to k3+k2−k1. As a function of t21 the echo amplitude decays due to scattering events, described by the dephasing time constant T2 [1].
Exciton Rabi oscillations and Rabi splitting differ significantly from their atomic counterparts in part because Coulomb interactions between excitons strongly influence the exciton Rabi frequency.' While both exciton Rabi oscillations and Rabi splitting were demonstrated recently in quantum wells (QWs),'.l experimental investigation of how exciton-exciton interactions affect these coherent optical Q~OCCSS~S has been hindered bya number of complications. In time-domain studies, the Rabi frequencyvaries with time due to the changing electric field strength. In typ ical spectral domain studies, a spectrally-broad probe pulse is spectrally resolved after its transmission through the sample. The resulting pump-probe spectra are difficult to interpret due to the presence of coherent spectral oscillations and a sensitive dependence on the pump-probe delay. In this paper we report studies of exciton Rabi splitting where spectrally narrow pump and probe pulses were used. In this case, coherent spectral oscillations in pump-probe spectra can be avoided by tuning the central frequency of the probe pulse. The intensity dependence of the Rabi splitting obtained from these studies reveals a distinctly nonlinear relationship between the Rabi frequency and the applied electric field, in contrast to the linear dependence expected from mean-field bed theoretical models.' Pump-probe experiments were performed on a 130 A GaAs1AlGa.k multiple QW sample at 10 K. Figure I shows results of pump-probe meas
We perform femtosecond spectrally resolved pump-probe differential reflectivity measurements on excitons in GaAs quantum wells in both coherent and incoherent regimes. The spectral signal is nonzero and oscillatory at $\ensuremath{-}\mathrm{ve}$ delay up to a few ps indicating persistent coherence between excitonic polarization induced by the probe pulse and the delayed pump pulse. The signal for small
+ve and $\ensuremath{-}\mathrm{ve}$ delay $(\ensuremath{\tau})$ shows modulation caused by quantum beats due to coexcitation of heavy and light hole excitons. The rise of the signal with $\ensuremath{\tau}$ for $\ensuremath{\tau}<0$ is rather nonexponential and is sensitive to detuning of the detection energy with respect to the exciton energy. The signal decay with $\ensuremath{\tau}$ for small
+ve $\ensuremath{\tau}$ shows dependence on pump-probe relative polarization. The excitonic reflectivity shows a large reduction caused by excitonic absorption saturation for both
+ve and $\ensuremath{-}\mathrm{ve}$ $\ensuremath{\tau}$ when the pump pulse intensity is increased to large values. To compare the experimental results with theory, we obtain an expression for the PPDR signal in terms of the third order excitonic polarization. This has an additional term not considered earlier to describe pump-probe experiments. The calculations are performed using optical Bloch equations, modified to incorporate exciton inhomogeneous broadening, quantum beats, and many body effects such as local field, excitation induced energy shift, and dephasing. These effects are found essential in explaining the observed PPDR spectral data. The delay dependence of the signal near the exciton energy is mainly controlled by inhomogeneous broadening for $\ensuremath{-}\mathrm{ve}$ $\ensuremath{\tau}.$ The signal decay for large
+ve $\ensuremath{\tau}$ has an exponential behavior determined by the lifetime of incoherent excitons. Experiments for collinear polarization reveal an additional exponential component for small
+ve delay. Theoretically, this is found to be related to exciton dephasing and is present only when many body effects are included.