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Optics Letters

Optical nonlinearities in AlxGa_1−xAs/GaAs asymmetric coupled quantum wells

Han Q. Le, J.V. Hryniewicz, W. D. Goodhue, V. A. Mims

Published Oct 1, 1988• 14 citations
Publisher

Abstract

Optical nonlinearities of Al(x)Ga(1-x)As/GaAs asymmetric coupled quantum wells within a p-i-n structure have been observed by using time-resolved spectroscopy. Under photoexcitation, exciton absorption lines exhibit spectral shifts of as much as approximately 1 meV. The recovery times of these spectral shifts are of the order of hundreds of picoseconds when the excitation photon is above the lowest exciton state but become less than 10 psec when excitation is below the lowest exciton state, indicating a virtual process. The behavior of these spectral shifts is consistent with the presence of a polarization induced by optical pumping. The polarization is believed to be due to the excitons that have nonvanishing electric dipole moments along the axis of the asymmetric coupled quantum wells.

DOI
10.1364/ol.13.000859

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Optical nonlinearities of Al(x)Ga(1-x)As/GaAs asymmetric coupled quantum wells within a p-i-n structure have been observed by using time-resolved spectroscopy. Under photoexcitation, exciton absorption lines exhibit spectral shifts of as much as approximately 1 meV. The recovery times of these spectral shifts are of the order of hundreds of picoseconds when the excitation photon is above the lowest exciton state but become less than 10 psec when excitation is below the lowest exciton state, indicating a virtual process. The behavior of these spectral shifts is consistent with the presence of a polarization induced by optical pumping. The polarization is believed to be due to the excitons that have nonvanishing electric dipole moments along the axis of the asymmetric coupled quantum wells.
We present here the first observation of quasisteady state optical nonlinearities in the absorption and photoluminescence (PL) spectra of GaAs/AlAs type II heterostructures. Using pump-probe spectroscopy we observed deep modulation, ΔT ~ 0.5 (Δα =−50,000 cm−1), due to a >40-meV blue shift and bleaching of the heavy hole exciton absorption peak. In addition, a blue shift of up to ~10 meV of the indirect PL line is observed with increasing PL excitation intensity. These nonlinearities are understood in terms of spatially separated layers of electrons and holes that are produced by the optical excitation process.
The nonlinear optical response of quantum well excitons is investigated experimentally using polarization resolved four wave mixing, optical-pump optical-probe, and optical-pump Terahertz-probe spectroscopy. The four-wave mixing data reveal clear signatures of coherent biexcitons which concur with straight-forward polarization selection rules at the Γ point. The type-I samples show the well-established time-domain beating signatures in the transients as well as the corresponding spectral signatures clearly. The latter are also present in type-II samples; however, the smaller exciton and biexciton binding energies in these structures infer longer beating times which, in turn, are accompanied by faster dephasing of the type-II exciton coherences. Furthermore, the THz absorption following spectrally narrow, picosecond excitation at energies in the vicinity of the 1s exciton resonance are discussed. Here, the optical signatures yield the well-established redshifts and blueshifts for the appropriate polarization geometries in type-I quantum well samples also termed “AC Stark Effect”. The THz probe reveals intriguing spectral features which can be ascribed to coherent negative absorption following an excitation into a virtual state for an excitation below the 1s exciton resonance. Furthermore, the scattering and ionization of excitons is discussed for several excitation geometries yielding control rules for elastic and inelastic quasiparticle collisions.
Linear, nonlinear and total optical absorption coefficients and relative refractive index changes for symmetric and asymmetric double V-shaped quantum well configurations formed within AlxGa1-xAs/GaAs heterostructure have been theoretically investigated. Responses of these coefficients to well widths, barrier widths and aluminium concentrations within the barrier as well as applied external electromagnetic fields were the subject of this study. The electronic spectra of the structures are obtained as a solution to the Schrödinger equation with relevant potential and external agents in the framework of effective mass and envelope wave function approximations. The optical properties are calculated by the analytical expressions obtained by iterative solutions within the compact density matrix approach. Although increasing barrier width and aluminium concentration act similarly significant red shifting on the referred coefficients for both symmetric and asymmetric double V-shaped wells, the varying well widths act differently for each configuration. Strengthening electric and magnetic fields shift the resonance peaks to blue for both symmetric and asymmetric wells. The results show that optical properties can be controlled by structural parameters, external probes and asymmetry of double V-shaped wells.
Abstract : In this paper we describe a detailed study of the complete time evolution of the optical nonlinearities of type-11 GaAs/AlAs quantum wells using nanosecond and femtosecond pump/probe spectroscopy. We explain these nonlinearities by solving the generalized Wannier equation for the case of a type-II quantum-well structure. In contrast to the usual type-I quantum-wells, we observe different shifts and saturations of light- and heavy-hole excitons as well as the absence of gain. The dominant effects are a blue shift and saturation of the heavy-hole (HH) exciton.
This dissertation presents investigations of fundamental optical nonlinearities in semi-conductor microstructures. Two distinct effects are studied. In the first part the excitonic optical Stark effect in InGaAs and GaAs multiple quantum-well structures is investigated by means of pump-probe spectroscopy. For nonresonant excitation below the excitonic transition the direction of the shift of the resonance depends on the polarization of the pump and probe pulses. In particular, for anti-circular polarization a surprising red-shift is observed. For resonant excitation, induced absorption energetically above and below the exciton transition and bleaching of the resonance is found. Experiments using both resonant and nonresonant excitation reveal the importance of bound and unbound two-exciton states in absorption changes of the 1s heavy-hole exciton resonance. It is found that higher-order Coulomb contributions determine the intensity as well as the time dependence of the differential excitonic absorption. In addition, the influence of light-hole excitons is analyzed. It is shown that the direction of the optical Stark shift for nonresonant excitation depends also sensitively on the heavy-hole to light-hole splitting and the detuning of the pump pulse. For very high pump intensities and nonresonant excitation the absorption is split when a circularly polarized pump and a linearly polarized probe beam are used. For co-circular excitation traces of hyper-Raman gain are observed. In the second part of this dissertation, the nonlinear optical response of semiconductor microcavities in the nonperturbative regime is studied in resonant single-beam transmission and pump-probe experiments. In both types of experiment, a pronounced third transmission peak lying spectrally between the two normal modes is observed. Its dependence on the probe intensity, pump intensity, pump-probe delay, exciton-cavity detuning and pump detuning is investigated. For single-beam transmission, the energy of the third peak parallels the position of the cavity resonance. It is more pronounced for circularly polarized excitation and lasts longer than the two normal modes. For pump-probe experiments, the third peak increases with decreasing probe intensity and increasing pump intensity. Its energy is close to the low-energy side of the pump spectrum and virtually unaffected by the cavity-exciton detuning. The appearance of the third peak requires temporal overlap of pump and probe pulses. The origin of this complex nonlinearity is the quantum nature of light, which induces intraband polarizations in the presence of a coherent driving field and a finite carrier density. It is found that the coupling of the intraband polarizations via guided modes to the polarization of the fundamental longitudinal mode is responsible for the third transmission peak. A fully quantized theory reproduces the experimental observations.
We have investigated intersubband absorptions between the conduction ground state and the first excited state of two AlxGa1−xAs/GaAs/AlxGa1−xAs multiple quantum well structures with x=0.3 and 85 Å well width, and with x=0.57 and 96 Å well width. Small-signal measurements show absorption peaks at 10.45 and 10.15 μm, respectively. Under an intense resonant excitation from a pulsed CO2 laser, saturation of the intersubband absorption occurred. The saturation intensity is estimated to be 340±120 kW/cm2 for the first sample and 375±120 kW/cm2 for the second. From these values, we have deduced subband decay times of the order of 10.6±3.5 ps for the first sample and 15.5±5 ps for the second.