Coherent effects in spectrally resolved pump-probe differential reflectivity measurements at exciton resonance in GaAs quantum wells

Abstract

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 $\ensuremath{\tau}l0$ 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.