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.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.

Physical review. B, Condensed matterSep 10, 20039 citations

Coherent signature of differential transmission signals in semiconductors: Theory and experiment

Georg Bartels, G. C. Cho, T. Dekorsy +3 more

Transient pump-probe signals of a GaAs/ ${\mathrm{Al}}_{\mathrm{x}}$ ${\mathrm{Ga}}_{1\mathrm{\ensuremath{-}}\mathrm{x}}$As quantum well are investigated both theoretically and experimentally for different excitation conditions. The calculations are based on a microscopic density-matrix approach taking higher-order correlations into account. We present spectrally resolved transients which provide insights into the nature of the differential transmission change. Especially the complex phase signature of heavy-hole--light-hole quantum beats in dependence of the detection energy allows for an identification of different microscopic processes in the pump-probe signal. The theoretical results are verified experimentally by comparison with the coherent and incoherent parts of the time-resolved data. We find a dominant role of the Coulomb-induced correlations up to the ${\mathrm{\ensuremath{\chi}}}^{(3)}$ relevant four-point level in the coherent signature in comparison to the Pauli blocking contributions.Transient pump-probe signals of a GaAs/${\mathrm{Al}}_{\mathrm{x}}$${\mathrm{Ga}}_{1\mathrm{\ensuremath{-}}\mathrm{x}}$As quantum well are investigated both theoretically and experimentally for different excitation conditions. The calculations are based on a microscopic density-matrix approach taking higher-order correlations into account. We present spectrally resolved transients which provide insights into the nature of the differential transmission change. Especially the complex phase signature of heavy-hole--light-hole quantum beats in dependence of the detection energy allows for an identification of different microscopic processes in the pump-probe signal. The theoretical results are verified experimentally by comparison with the coherent and incoherent parts of the time-resolved data. We find a dominant role of the Coulomb-induced correlations up to the ${\mathrm{\ensuremath{\chi}}}^{(3)}$ relevant four-point level in the coherent signature in comparison to the Pauli blocking contributions.

Physical review. B, Condensed matterJun 15, 199765 citations

Pump-Probe Spectroscopy — Revisited

P. R. Berman

Springer eBooksJan 1, 20000 citations

Time-resolved 3D imaging of ultrafast spin–orbit wave packet dynamics

Tim Bayer, Daniela Gräfing, Stefanie Kerbstadt +4 more

We combine bichromatic polarization pulse shaping with photoelectron imaging tomography for time-resolved spatial imaging of ultrafast spin–orbit wave packet (SOWP) dynamics in atoms. Polarization-shaped two-color pump-probe sequences are generated by spectral amplitude and phase modulation of a femtosecond input pulse and used to excite SOWPs in the potassium fine-structure doublet. By selecting different spectral bands for pump and probe pulse, we achieve interference-free detection of the spatiotemporal SOWP dynamics. Using tomographic techniques, we reconstruct the three-dimensional photoelectron momentum distribution (3D-ED) created by the probe pulse. Time-resolved measurement of the 3D-ED reveals the orbital realignment dynamics induced by spin–orbit interaction in the neutral atom.We combine bichromatic polarization pulse shaping with photoelectron imaging tomography for time-resolved spatial imaging of ultrafast spin–orbit wave packet (SOWP) dynamics in atoms. Polarization-shaped two-color pump-probe sequences are generated by spectral amplitude and phase modulation of a femtosecond input pulse and used to excite SOWPs in the potassium fine-structure doublet. By selecting different spectral bands for pump and probe pulse, we achieve interference-free detection of the spatiotemporal SOWP dynamics. Using tomographic techniques, we reconstruct the three-dimensional photoelectron momentum distribution (3D-ED) created by the probe pulse. Time-resolved measurement of the 3D-ED reveals the orbital realignment dynamics induced by spin–orbit interaction in the neutral atom.

New Journal of PhysicsJan 2, 201921 citations

+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.

Transient pump-probe signals of a GaAs/

{\mathrm{Al}}_{\mathrm{x}}

${\mathrm{Ga}}_{1\mathrm{\ensuremath{-}}\mathrm{x}}$As quantum well are investigated both theoretically and experimentally for different excitation conditions. The calculations are based on a microscopic density-matrix approach taking higher-order correlations into account. We present spectrally resolved transients which provide insights into the nature of the differential transmission change. Especially the complex phase signature of heavy-hole--light-hole quantum beats in dependence of the detection energy allows for an identification of different microscopic processes in the pump-probe signal. The theoretical results are verified experimentally by comparison with the coherent and incoherent parts of the time-resolved data. We find a dominant role of the Coulomb-induced correlations up to the ${\mathrm{\ensuremath{\chi}}}^{(3)}$ relevant four-point level in the coherent signature in comparison to the Pauli blocking contributions.