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Physical review. B, Condensed matter

Observation of the ultrafast two-photon coherent biexciton oscillation in a GaAs / Al x Ga 1 − x As multiple quantum well

Kyle B. Ferrio, Duncan G. Steel

Published Aug 15, 1996• 31 citations
Publisher

Abstract

Polarization-dependent heterodyne four-wave-mixing measurements with a phase-conjugate Michelson interferometer reveal a macroscopic nonradiative 770-THz oscillation in the nonlinear optical susceptibility of GaAs multiple quantum wells. The oscillation is interpreted as the temporal evolution of the two-photon nonradiative biexcitonic coherence.

DOI
10.1103/physrevb.54.r5231

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Optically induced coherences reveal key features of nonlinearities in the optical response of semiconductors and can be employed to obtain information about dynamical processes via such techniques as transient four-wave mixing and differential transmission. This thesis presents experimental observations of three previously unrecognized aspects of coherent nonlinear optical phenomena occurring in gallium arsenide and multiple quantum wells: excitation-induced dephasing, two-photon biexcitonic coherence, and electronic Raman coherence. Results are analyzed using optical Bloch equations, which emphasize the potential generalization to other semiconductor systems. Excitation-induced dephasing is similar to classical line broadening. The work in this thesis shows for the first time that this incoherent effect is directly responsible for the dominant coherent optical nonlinearity in bulk gallium arsenide. Exact analytic models show that excitation-induced dephasing accounts for the previously unexplained polarization and density dependence of four-wave mixing signals obtained at the 1s exciton resonances in gallium arsenide. This thesis also presents the first observation of the two-photon biexcitonic coherence in a gallium arsenide multiple quantum well using a modified Michelson phase-conjugate interferometer to directly observe the 770-Terahertz oscillation of the nonradiative superposition of the electronic ground state and the biexciton state. The contribution of the two-photon coherence to the nonlinear optical response is thereby confirmed, in addition to the well-known stepwise biexcitonic response. Finally, the short-lived electronic Raman coherence between the light- and heavy-hole 1s excitons in gallium arsenide is conclusively demonstrated for the first time. The Raman coherence provides direct access to dephasing processes not detectable in conventional linear spectroscopy. Similar non-radiative coherences are related to population trapping, electromagnetically induced transparency, and lasing without inversion in atomic systems, and the new observations in gallium arsenide suggest that analogous phenomena may occur in semiconductors.

•Jan 1, 1996•0 citations
Polarization-dependent heterodyne four-wave-mixing measurements with a phase-conjugate Michelson interferometer reveal a macroscopic nonradiative 770-THz oscillation in the nonlinear optical susceptibility of GaAs multiple quantum wells. The oscillation is interpreted as the temporal evolution of the two-photon nonradiative biexcitonic coherence.
We report measurements of two-photon transitions to the biexciton state and exciton-biexciton transitions (M band) in GaAs/Alx{\mathrm{Al}}_{\mathit{x}}Alx​${\mathrm{Ga}}_{1\mathrm{\ensuremath{-}}\mathit{x}}$As multiple quantum wells by spectrally resolving the self-diffraction in a four-wave-mixing experiment. Furthermore, nonlinear quantum beats between a coherently prepared population of excitons and biexcitons are observed. The analysis yields a binding energy of 1.8 meV for the biexciton in 116-A\r{} quantum wells.
We present in this paper polarization dependent four-wave-mixing (FWM) measurements in homogeneously broadened GaAs quantum wells (QW). We have unambiguously demonstrated the important contribution of the two-photon coherence (TPC) between the ground and biexciton states to the nonlinear response. We show for the first time the dominant effects of the TPC on the polarization dependence of FWM. In particular, by including the TPC-induced contribution, we are able to account for the anomalous polarization dependence, a subject of considerable current interest [1].
We investigate the spectral properties of the excitonic nonlinear response in a GaAs quantum-well sample containing wells of different thicknesses. We observe both the heavy-hole biexciton and the light-hole biexciton in the transient four-wave mixing spectrum and estimate their binding energy dependence on well width. For moderate excitation densities the signal for negative delay at the heavy-hole exciton and biexciton resonances is due to two-photon transitions to the biexciton states through the exciton states. The temporal behavior of the transient four-wave mixing signal from the heavy-hole exciton resonance is strongly dependent on the spectral position of the laser. We show that this effect is due to interference phenomena and to excitation-induced dephasing.
We report time-resolved degenerate four-wave-mixing experiments on a high-quality single GaAs quantum well. The signals for parallel and cross-polarized exciting pulses show pronounced quantum beats with different frequencies corresponding to the heavy/light-hole splitting and the biexciton binding energy, respectively. Comparison of the experimental data with solutions of the optical Bloch equations for a phenomenological model system shows that these features result from strong contributions of the biexcitonic state. The importance of biexcitons to the nonlinear coherent response of the two-dimension exciton is further confirmed by the frequency dependence of the time-integrated four-wave-mixing signal amplitudes measured for the two polarization geometries.
By degenerate four-wave mixing experiments in a two-beam geometry, we have investigated the initial coherence and dephasing of quasi two-dimensional excitions and biexcitons in GaAs multiple quantum wells. The dephasing has contributions from phonon scattering, interface-roughness scattering and exciton-exciton scattering. Inhomogeneous broadening and generation of coherent wavepackets play a significant role in the coherent exciton dynamics. The incoherent exciton dynamics, diffusion and recombination, is studied by three-beam transient grating experiments. A significant difference in the interface roughness scattering of coherent and incoherent (thermalized) excitons is observed.
Optically induced coherences reveal key features of nonlinearities in the optical response of semiconductors and can be employed to obtain information about dynamical processes via such techniques as transient four-wave mixing and differential transmission. This thesis presents experimental observations of three previously unrecognized aspects of coherent nonlinear optical phenomena occurring in gallium arsenide and multiple quantum wells: excitation-induced dephasing, two-photon biexcitonic coherence, and electronic Raman coherence. Results are analyzed using optical Bloch equations, which emphasize the potential generalization to other semiconductor systems. Excitation-induced dephasing is similar to classical line broadening. The work in this thesis shows for the first time that this incoherent effect is directly responsible for the dominant coherent optical nonlinearity in bulk gallium arsenide. Exact analytic models show that excitation-induced dephasing accounts for the previously unexplained polarization and density dependence of four-wave mixing signals obtained at the 1s exciton resonances in gallium arsenide. This thesis also presents the first observation of the two-photon biexcitonic coherence in a gallium arsenide multiple quantum well using a modified Michelson phase-conjugate interferometer to directly observe the 770-Terahertz oscillation of the nonradiative superposition of the electronic ground state and the biexciton state. The contribution of the two-photon coherence to the nonlinear optical response is thereby confirmed, in addition to the well-known stepwise biexcitonic response. Finally, the short-lived electronic Raman coherence between the light- and heavy-hole 1s excitons in gallium arsenide is conclusively demonstrated for the first time. The Raman coherence provides direct access to dephasing processes not detectable in conventional linear spectroscopy. Similar non-radiative coherences are related to population trapping, electromagnetically induced transparency, and lasing without inversion in atomic systems, and the new observations in gallium arsenide suggest that analogous phenomena may occur in semiconductors.