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Nonlinear optical processes in semiconductor microcavities and sodium vapor

David Wick

Published Jan 1, 1997• 1 citation
OpenAlex

Abstract

Nonlinear optical phenomena in both semiconductor microcavities and sodium vapor are investigated. Systems displaying atomic and excitonic coupling are studied in detail in order to unravel underlying physical principles. Possible applications for these systems are evaluated where appropriate. Normal-mode coupling (NMC) in a semiconductor microcavity is achieved when a narrow-linewidth quantum well exciton resonance is coincident with the cavity mode of a high-finesse microcavity. This interaction leads to a double-peaked spectrum in either transmission, reflection, or photoluminescence (PL). The high-quality microcavities studied here at liquid-Helium temperatures reveal intensity dependent behavior that has not previously been observed. Nonlinear saturation of the exciton leads to a spectral broadening of the excitonic absorption without a significant loss in oscillator strength. This results in a reduction of the two transmission peaks with almost no change in the splitting between the peaks. Such behavior is easily explained using phenomenological nonlinear dispersion theory. In this nonlinear regime, the luminescence from the microcavity shows a gradual transition from the nonperturbative regime of NMC to lasing with increasing excitation. The observed behavior is explained by density-dependent changes in both the transmission of the microcavity and the bare-exciton emission, rather than a boson-condensation of excitons which has been previously proposed. An intermediate-finesse microcavity also modifies the emission distribution from a bulk-semiconductor at room temperature. Angularly resolved emission spectra and quantum efficiency measurements show the PL is strongly dependent on the reflectivity of the microcavity. Unfortunately, the enhancement in the decay rate of excitons due to high-reflectivity mirrors seen previously by our group does not result in an increased quantum efficiency. High-gain optical-wavefront amplification in atomic sodium vapor is demonstrated via both the three-photon effect and stimulated Raman scattering (SRS). In both cases, single-pass weak-field gain of nearly 400 is achieved with only 800 mW of pump power near 589 nm. In the case of SRS, phase preservation of the amplified wavefront, which is necessary in adaptive imaging applications, is also demonstrated.

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International Conference on Ultrafast Phenomena•Jan 1, 1996•0 citations
Nonlinear optical phenomena in both semiconductor microcavities and sodium vapor are investigated. Systems displaying atomic and excitonic coupling are studied in detail in order to unravel underlying physical principles. Possible applications for these systems are evaluated where appropriate. Normal-mode coupling (NMC) in a semiconductor microcavity is achieved when a narrow-linewidth quantum well exciton resonance is coincident with the cavity mode of a high-finesse microcavity. This interaction leads to a double-peaked spectrum in either transmission, reflection, or photoluminescence (PL). The high-quality microcavities studied here at liquid-Helium temperatures reveal intensity dependent behavior that has not previously been observed. Nonlinear saturation of the exciton leads to a spectral broadening of the excitonic absorption without a significant loss in oscillator strength. This results in a reduction of the two transmission peaks with almost no change in the splitting between the peaks. Such behavior is easily explained using phenomenological nonlinear dispersion theory. In this nonlinear regime, the luminescence from the microcavity shows a gradual transition from the nonperturbative regime of NMC to lasing with increasing excitation. The observed behavior is explained by density-dependent changes in both the transmission of the microcavity and the bare-exciton emission, rather than a boson-condensation of excitons which has been previously proposed. An intermediate-finesse microcavity also modifies the emission distribution from a bulk-semiconductor at room temperature. Angularly resolved emission spectra and quantum efficiency measurements show the PL is strongly dependent on the reflectivity of the microcavity. Unfortunately, the enhancement in the decay rate of excitons due to high-reflectivity mirrors seen previously by our group does not result in an increased quantum efficiency. High-gain optical-wavefront amplification in atomic sodium vapor is demonstrated via both the three-photon effect and stimulated Raman scattering (SRS). In both cases, single-pass weak-field gain of nearly 400 is achieved with only 800 mW of pump power near 589 nm. In the case of SRS, phase preservation of the amplified wavefront, which is necessary in adaptive imaging applications, is also demonstrated.
Different aspects of the photoluminescence from semiconductor quantum-confined structures are studied in this dissertation, for a better understanding of fundamental physics of semiconductors.The precursor of any photoluminescence study is the characterization of the linear optical properties of the semiconductor structure. High resolution absorption measurements were performed in order to study the interplay of disorder and acoustic phonon scattering in a quantum well. Also, reflectivity measurements, together with a fitting procedure based on the transfer matrix formalism, are used to determine the thickness of samples.Excitons are atom-like quasi-particles, formed from a bound electron-hole pair. They follow a Bose-Einstein statistic, so in principle it is possible to achieve an excitonic Bose-Einstein condensate. Time resolved photoluminescence measurements were performed over an extensive range of lattice temperatures and carrier concentrations, in order to determine the fraction of excitons formed from the electron-hole plasma in a quantum well, after non-resonant excitation. The experimental spectra were compared to a pure plasma calculation first, then excitons were taken into account. The highest fraction of formed excitons is found for low temperatures and intermediate carrier densities. This fraction is found to be very small, and this has clear implications on the excitonic Bose-Einstein condensation studies.The photoluminescence emitted left and right from a quantum well is interfered in a modified Mach-Zender interferometer. It is shown that the light emitted on the two paths will interfere for a V-shape geometry and will not for any other paths.A structure formed by placing a quantum well in a field antinode of a resonant planar microcavity exhibits normal mode coupling: splitting of the resonance spectral line. The coherence properties of the photoluminescence from a normal-mode-coupling microcavity are studied using another version of the Mach-Zender interferometer. The degree of coherence measured in this way depends greatly on the pump wavelength and intensity, ranging from zero to 0.8. However, direct observation of the emission speckle shows significant coherence in all cases. The difference is explained by the different methods used to evaluate the coherence.The strong coupling between a quantum dot and a photonic crystal nanocavity is investigated by observation of photoluminescence. A new method of tunning the cavity wavelength by deposition of a thin film of solid Xenon on all the surfaces of the sample is presented. The method allows the scanning of the cavity wavelength with about 5 nm without a decrease in the quality factor and without changing the temperature.Finally, an extensive study of the quality factors of quantum dot photonic crystal nanocavities is presented. The role of the quantum dot ensemble absorption is investigated. At higher excitation levels, lasing is observed and discussed.
Recently, several research groups have reported investigations of vacuum-field Rabi splittings (VRS) in the linear response of strongly coupled semiconductor microcavities [1-4]. We have previously reported on the dynamics of time-domain vacuum Rabi oscillations, which are most easily understood in the framework of cavity exciton-polaritons, in which the in-plane momentum k|| is conserved [2], so that at each k|| a single cavity mode interacts with only a single mode of the electromagnetic field (Jaynes-Cummings model). In high Q semiconductor microcavities, the strong coupling between two-dimensional excitons and planar distributed- Bragg-reflector cavity modes results in several-meV splittings observable in the reflectivity or absorption spectrum. In the low excitation regime, the VRS is independent of light intensity incident on the cavity, since the vacuum-Rabi frequency exceeds the externally-driven Rabi frequency (in which case the Jaynes-Cummings model is equivalent to the linear dispersion of the coupled exciton-cavity system). As the incident light intensity is increased, two different effects may be expected to contribute to the nonlinear response. First, as long as the excitonic absorption is equivalent to a two-level system, higher-lying states of the Jaynes-Cummings ladder might be observable. Second, at high intensity phase-space filling and Coulomb screening of the exciton states results in a reduced oscillator strength which leads to a reduced VRS; this effect has no analogue in the case of atom-cavity systems. In this paper, we apply several ultrafast nonlinear techniques to investigate the nonlinear response of semiconductor microcavities.
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.
The normal modes in a nonperturbatively coupled quantum-well semiconductor microcavity are linear superpositions of the QW exciton and cavity mode when the QW exciton transition is resonant with the cavity mode. When the lower normal mode is excited by a phase-locked pair of optical pulses, the nonlinear response of a probe pulse tuned to the upper mode is controlled. Thus the normal modes are coupled in their nonlinear optical response due to the nonlinearity of the exciton underlying the two normal modes. The cavity enhancement of the excitonic nonlinearity gives rise to a large signal; modulating the relative phase of the excitation pulses produces a differential reflectivity of up to 10%. Besides the coherent control of normal modes which is explainable with in the frame of semiclassical models, we observe a purely quantum mechanical phenomenon in our system. The quantum correlations between the field and carrier density lead to intraband coherences which live much longer than the interband dephasing time.
Semiconductor quantum microcavities are interesting physical systems in which fundamental interactions between light and excitons can be explored. For example, in the weak - coupling limit, modified excitonic spontaneous emission can be observed. In the strong-coupling limit, the cavity field modes and the quantum well exciton modes become coupled; the normal modes of the system are "cavity-polaritons" [1,2]. For in-plane wavevectors k// near zero, the normal modes are split by the dipole coupling between the excitons and the cavity vacuum field. This splitting is often referred to as a vacuum-Rabi splitting (VRS), as it has the same physical origin as the VRS observed in the interactions of atoms with single-mode cavities. The physical system in this work consists of a λ planar microcavity formed by two distributed-Bragg reflectors, with five GaAs quantum wells situated in the center of the cavity. In all the experiments described here, the exciton and cavity modes are on resonance (the low-field VRS is 6 meV for this sample).