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Physical review. B, Condensed matter

Interaction-induced effects in the nonlinear coherent response of quantum-well excitons

Hans Peter Wagner, A. Schätz, W. Langbein, J. M. Hvam, Arthur L. Smirl

Published Aug 15, 1999• 45 citations
Publisher

Abstract

Interaction-induced processes are studied using the third-order nonlinear polarization created in polarization-dependent four-wave-mixing experiments (FWM) on a ZnSe single quantum well. We discuss their influence by a comparison of the experimental FWM with calculations based on extended optical Bloch equations including local-field effects, excitation-induced dephasing, and biexciton formation. The investigations show that, for copolarized input fields, excitation-induced dephasing is the dominant FWM mechanism, followed by the conventional density-grating FWM process, biexcitonic contributions, and local-field effects. For cross-linear polarized input fields the excitation-induced dephasing mechanism is canceled so that the conventional density-grating FWM process and biexcitonic contributions are dominating.

DOI
10.1103/physrevb.60.4454

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Interaction-induced processes are studied using the third-order nonlinear polarization created in polarization-dependent four-wave-mixing experiments (FWM) on a ZnSe single quantum well. We discuss their influence by a comparison of the experimental FWM with calculations based on extended optical Bloch equations including local-field effects, excitation-induced dephasing, and biexciton formation. The investigations show that, for copolarized input fields, excitation-induced dephasing is the dominant FWM mechanism, followed by the conventional density-grating FWM process, biexcitonic contributions, and local-field effects. For cross-linear polarized input fields the excitation-induced dephasing mechanism is canceled so that the conventional density-grating FWM process and biexcitonic contributions are dominating.
Spectrally resolved and time-integrated degenerate four-wave mixing (FWM) experiments with ultra-short pulses have been used to investigate the relaxation times and coherent interactions of excitons in the Boltzmann and in the quantum kinetic regime in ZnSe single quantum wells.Three-pulse FWM experiments using 100 fs pulses in a 10 nm thick ZnSe/ZnMgSe single quantum well reveal nearly equal zero-density dephasing rates for coherences between + σ and - σ heavy-and/or light-hole exciton states as compared to the dephasing rate of the interband coherence between these states and the ground state.The measurements also demonstrate that exciton-exciton scattering destroys the phase coherence between heavy-and light-hole excitons about three times more effectively than the coherence between + σ and + σ heavy-hole excitons.The different coherent nonlinear signals obtained in a three-beam FWM experiment are explained and reproduced by numerical calculations of the optical Bloch equations for a ten-level model including excitation induced dephasing (EID).Two-beam FWM experiments using 30 fs pulses on a 10 nm ZnSe quantum well reveal marked quantum beats and a pronounced non-exponential decay for delay times smaller ~500 fs.The pronounced peak at pulse overlap is attributed to rapid destructive interference of the created polarization and to spin dependent quantum kinetic effects caused by the transient formation of an electron-hole (eh) pair grating.The three-beam FWM trace shows a bi-exponential decay which is attributed to a nonlinear polarization that is caused by the interaction of polarization 3 k with both an exciton grating and an eh-pair grating.Model calculations using the OBEs of a two level system that includes ∑ -+
The coherent response of excitons in semiconductor nanostructures measured in four-wave mixing (FWM) depends strongly on the inhomogeneous broadening of the exciton transition. We investigate GaAs/Al0.3Ga0.7As single quantum wells (SQW) and AlxGa1-xAs mixed crystals. Additional to the usual phase-space filling nonlinearity, excitation-induced dephasing (EID) and biexciton formation (BIF) are important. EID leads to a strong dependence of the signal on the angle between the linear input polarizations. We find that EID persists in inhomogeneous systems, showing that the mutual density-dependent dephasing rate difference between two subsystems within the inhomogeneous distribution is strongly dependent on their energy difference. BIF is strongly affecting the cross-linear polarized FWM response. The signal for positive delay is dominated by the transitions from the one-exciton state X to the two-exciton states. Here, the third-order polarization at X-XX is not at the same resonance as the first-order polarization at 0-X. Consequently, the rephasing of the microscopic third-order polarization to the macroscopic FWM photon echo is blurred by the non-perfect correlation of X and XX energies, leading to a fast and non-exponential signal decay in delay time. For inhomogeneous broadenings larger than the biexciton binding energy, we find an enhanced biexciton binding energy, and a quenching of the oscillator strength of the unbound biexciton.
We investigate interband coherences as well as coherences between ${\ensuremath{\sigma}}^{+}$ and ${\ensuremath{\sigma}}^{\ensuremath{-}}$ exciton states in a 10 nm thick ZnSe/ZnMgSe single quantum well by spectrally resolved three-pulse degenerate four-wave mixing using circularly polarized 100 fs pulses. Polarization and intensity dependent measurements are performed to identify the coherent processes responsible for the nonlinear signal into the ${\mathbf{k}}_{3}+{\mathbf{k}}_{2}\ensuremath{-}{\mathbf{k}}_{1}$ direction and to study the influence of Coulomb scattering on the dephasing rates. The experiments reveal nearly equal zero-density dephasing rates for coherences between ${\ensuremath{\sigma}}^{+}$ and ${\ensuremath{\sigma}}^{\ensuremath{-}}$ heavy- and/or light-hole exciton states as compared to the dephasing rate of the interband coherence between these states and the ground state. The measurements also demonstrate that exciton--exciton scattering destroys the phase coherence between heavy- and light-hole excitons about three times more effectively than the coherence between ${\ensuremath{\sigma}}^{+}$ and ${\ensuremath{\sigma}}^{\ensuremath{-}}$ heavy-hole excitons. The characteristic features of the experimental results are explained and reproduced by numerical calculations of the optical Bloch equations for a ten-level model including excitation induced dephasing.
Summary form only given.The coherent response of excitons in semiconductor nanostructures, as measured in four wave mixing (FWM) experiments, depends strongly on the inhomogeneous broadening of the exciton transition. We investigate GaAs-AlGaAs single quantum wells (SQW) of 4 nm to 25 nm well width. Two main mechanisms are found to be important. First, the excitation-induced dephasing FWM signal (EID), which leads to a strong dependence of the signal on the angle between the linear input polarizations. The presence of the EID in the mainly homogeneously broadened sample (25 nm) is shown by the beating between EID and two-photon coherence (TPC) at the exciton for negative delay and co-linear polarized excitation. It vanishes for cross-polarized excitation, thus excluding the importance of local-field effects.