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Quantum Electronics and Laser Science Conference

Polarization selection rules for degenerate four-wave mixing on 2D excitons

J. Kühl, Richard Eccleston, E. J. Mayer, D. Bennhardt, P. Thomas

Published May 2, 1993• 0 citations
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Abstract

Several recent two-pulse degenerate four- wave-mixmg experiments on 2D excitons in GaAs showed considerably faster dephasing rates for cross-polarized beams than for colinear polarization.1,2 Moreover, time-resolved analysis of the DFWM signal on some samples revealed a photon echo and a free-induction decaylike behavior for the parallel and perpendicular polarizations, respectively.1

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Several recent two-pulse degenerate four- wave-mixmg experiments on 2D excitons in GaAs showed considerably faster dephasing rates for cross-polarized beams than for colinear polarization.1,2 Moreover, time-resolved analysis of the DFWM signal on some samples revealed a photon echo and a free-induction decaylike behavior for the parallel and perpendicular polarizations, respectively.1
In degenerate four-wave-mixing (DFWM) experiments the polarization of the incident laser pulses can have a strong influence on the measured signal. For GaAs quantum wells a number of DFWM experiments were performed by using either parallel or perpendicular polarization of the incident laser pulses. Experimentally, it turned out that some characteristic features of the signal differ appreciably for the two configurations. In particular, different dephasing times, phase shifts of the quantum beats, different time-resolved behavior (echoes versus free-induction decay), and intensity dependence of the measured signal have been reported.1–3
We report the experimental results of two-pulse transient four-wave mixing near the first heavy-hole quantum-well exciton. Input pulses with similar polarizations (circular or linear) measure the exciton dephasing rate; opposite circular polarized pulses produce no four-wave mixing signal, while crossed linear polarized pulses generate a weaker signal with a faster dephasing rate. This signal is attributed to the biexcitonic transition, which was directly observed in a separate nondegenerate four-wave mixing experiment. The selection rules for these transitions are discussed and confirm the treatment of the excitonic transition as a three-level system.
We have studied picosecond two-pulse degenerate four-wave mixing in GaAs/AlAs quantum wells under different polarization configurations of the two pump beams and the analyzed optical polarization. We observe two components, a prompt free polarization decay (FPD) and a delayed photon echo (PE), which show different polarization rules and dephasing times. The observed polarization rules are consistently explained in a theoretical model. Within this model, the two-component behavior is a direct consequence of short-range disorder. The PE dephasing rate is associated with the homogeneous broadening of the excitons while the FPD corresponds to the total dephasing rate, consisting of the homogeneous and inhomogeneous (short-range and long-range) broadenings.
Recent transient four-wave-mixing experiments in the two-pulse photon-echo configuration performed on GaAs quantum wells have yielded the surprising result that in some samples the T2{\mathit{T}}_{2}T2​ time obtained from the polarization decay can be shorter for cross-polarized input fields than for parallel input fields. A concomitant change from photon-echo to free-induction-decay behavior has also been observed. A phenomenological model is presented which explains these observations by means of a disorder-induced coupling of the ${\mathrm{\ensuremath{\sigma}}}^{+}$ and ${\mathrm{\ensuremath{\sigma}}}^{\mathrm{\ensuremath{-}}}$ exciton transitions which is inhomogeneous in coupling strength. Such coupling also leads to a remarkable change in the light-hole--heavy-hole exciton quantum beat phase as a function of pulse delay for a critical relative orientation of the polarization of the incident pulses. Experimental observations of this effect are presented to support the validity of the model.
The exciton coherent signal decay rate in GaAs quantum wells, as measured in four-wave mixing experiments, depends on the polarization of the excitation pulses. Using polarization-dependent two-dimensional coherent spectroscopy, we show that this behavior is due to the bosonic character of excitons. Interference between two different quantum mechanical pathways results in a smaller decay rate for cocircular and colinear polarization of the optical excitation pulses. This interference does not exist for cross-linearly polarized excitation pulses resulting in a larger decay rate. Our result shows that the bosonic nature of excitons must be considered when interpreting ultrafast spectroscopic studies of exciton dephasing in semiconductors. This behavior should be considered while interpreting results of ultrafast spectroscopy experiments involving bosonlike excitations.