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This Master’s dissertation focuses on exploring optical nonlinearities in IIIV semiconductors. This work covers a range of III-V materials and a few devices. To begin with, optical characterization of Aluminium Gallium Arsenide (AlGaAs) waveguides with enhanced nonlinear optical interactions was carried out. We have experimentally demonstrated wide conversion ranges andhigh conversion efficiencies for four-wavemixing inAlGaAswaveguides with three different geometries. In addition to that, both linear and nonlinear losses in each of these geometries were explored. AlGaAs represents only one compound of the large group of III-V semiconductors. To explore the potentials of other semiconductors compounds of this group for nonlinear optics, it is imperative to have information about refractive indices of different III-V compounds. This refractive index information is only available for some binary compounds in isolated spectral windows. In this thesis, we developed a model capable of predicting the values of the refractive indices of binary, ternary and quaternary III-V semiconductor compounds from the values of their band-gap energies. We compared the value predicted by our proposed model with existing experimental data and it was found not only is the predicted values in good agreement with the known values, but also has a lower error margin when compared to previously reported models. Finally, in quest for more suitable material platform for nonlinear photonic integration at different wavelength ranges, a detailed analysis of other potential III-V compounds not previously explored for photonic integration is presented.

We correlated experimental results with theoretical estimations of the dielectric function ε(ω) in two contexts: the effect of an electric field in quantum wells and that of the spin polarization of an interacting electron-hole plasma in bulk semiconductors. In the first part, we recorded photoreflectance spectra from Ge/GeSi quantum wells of different widths but having comparable builtin electric fields caused by doping. The reason why the spectra differed in overall shape was difficult to understand by conventional methods, for example, by calculating the allowed transition energies or by fitting the data with lineshape functions at each transition energy. Instead, we computed the photoreflectance spectra from first-principles by using the confined electron and hole wavefunctions. This method showed that the spectra differ in overall shape because of the experimentally hitherto unobserved trend in quantum well electro-optical properties, from the quantum confined Franz-Keldysh effect to the bulk Franz-Keldysh effect, as the well width is increased. The second part develops a threeband microscopic theory for the optical properties due to spin-polarized carriers in quasiequilibrium. We show that calculations based on this theory reproduce all the trends observed in a recent circularly polarized pump-probe experiment reported in the literature. To make the computation less intensive, we proposed a simplified, two-band version of this theory which captured the main experimental features. Besides, we constructed a cw diode laser-based pump-probe setup for our own optical studies of spin-polarized carriers by Kerr rotation. We achieved a sensitivity of detection of Kerr rotation of 3 x 10¯ 8 rad, corresponding to an order of magnitude improvement over the best reports in the literature. The efficacy of our setup allowed for the demonstration of a pumpinduced spin polarization in bulk GaAs, under the unfavorable conditions of steady-state and room temperature.

Bragg reflection waveguides (BRW) or one-dimensional photonic bandgap structures have been demonstrated for phase-matching chi(2) nonlinearities in AlxGa1-xAs. The method exploits strong modal dispersion of a Bragg mode and total internal reflection modes co-propagating inside the waveguide. It is shown that phase-matching is attained among the lowest order modes of interacting harmonics, which allows maximizing the utilization of harmonics powers for nonlinear interactions. As our first demonstration, we report second-harmonic generation (SHG) of a 2-ps telecommunication pump in a 2.4 mm long slab BRW. The conversion efficiency is estimated as 2.0 %/W.cm^2 with a generated SH power of 729 nW. This efficiency has been considerably improved by introducing lateral confinement of optical modes in ridge structures. Characterizations denote that efficiency of SHG in ridge BRWs can increase by over an order of magnitude in comparison to that of the slab device. Also, we report continuous-wave SHG in BRWs. Using a telecommunication pump with a power of 98 mW, the continuous-wave SH power of 23 nW is measured in a 2.0 mm long device. Significant enhancements of chi(2) interactions is obtained in the modified design of matching-layer enhanced BRW (ML-BRW). For the first time, we report type-II SHG in ML-BRW, where the second-harmonic power of 60 µW is measured for a pump power of 3.3 mW in a 2.2 mm long sample. Also, we demonstrate the existence of type-0 SHG, where both pump and SH signal have an identical TM polarization state. It is shown that the efficiency of the type-0 process is comparable to type-I and type-II processes with the phase-matching wavelengths of all three interactions lying within a spectral window as small as 17 nm. ML-BRW is further reported for sum-frequency and difference-frequency generations. For applications requiring high pump power, a generalized ML-BRW design is proposed and demonstrated. The proposed structure offsets the destructive effects of third-order nonlinearities on chi(2) processes when high power harmonics are involved. This is carried out through incorporation of larger bandgap materials by using high aluminum content AlxGa1-xAs layers without undermining the nonlinear conversion efficiency. Theoretical investigations of BRWs as integrated sources of photon-pairs with frequency correlation properties are discussed. It is shown that the versatile dispersion properties in BRWs enables generation of telecommunication anti-correlated photon-pairs with bandwidth tunablity between 1 nm and 450 nm.

Bragg reflection waveguides (BRW) or one-dimensional photonic bandgap structures have been demonstrated for phase-matching chi(2) nonlinearities in AlxGa1-xAs. The method exploits strong modal dispersion of a Bragg mode and total internal reflection modes co-propagating inside the waveguide. It is shown that phase-matching is attained among the lowest order modes of interacting harmonics, which allows maximizing the utilization of harmonics powers for nonlinear interactions. As our first demonstration, we report second-harmonic generation (SHG) of a 2-ps telecommunication pump in a 2.4 mm long slab BRW. The conversion efficiency is estimated as 2.0 %/W.cm^2 with a generated SH power of 729 nW. This efficiency has been considerably improved by introducing lateral confinement of optical modes in ridge structures. Characterizations denote that efficiency of SHG in ridge BRWs can increase by over an order of magnitude in comparison to that of the slab device. Also, we report continuous-wave SHG in BRWs. Using a telecommunication pump with a power of 98 mW, the continuous-wave SH power of 23 nW is measured in a 2.0 mm long device. Significant enhancements of chi(2) interactions is obtained in the modified design of matching-layer enhanced BRW (ML-BRW). For the first time, we report type-II SHG in ML-BRW, where the second-harmonic power of 60 µW is measured for a pump power of 3.3 mW in a 2.2 mm long sample. Also, we demonstrate the existence of type-0 SHG, where both pump and SH signal have an identical TM polarization state. It is shown that the efficiency of the type-0 process is comparable to type-I and type-II processes with the phase-matching wavelengths of all three interactions lying within a spectral window as small as 17 nm. ML-BRW is further reported for sum-frequency and difference-frequency generations. For applications requiring high pump power, a generalized ML-BRW design is proposed and demonstrated. The proposed structure offsets the destructive effects of third-order nonlinearities on chi(2) processes when high power harmonics are involved. This is carried out through incorporation of larger bandgap materials by using high aluminum content AlxGa1-xAs layers without undermining the nonlinear conversion efficiency. Theoretical investigations of BRWs as integrated sources of photon-pairs with frequency correlation properties are discussed. It is shown that the versatile dispersion properties in BRWs enables generation of telecommunication anti-correlated photon-pairs with bandwidth tunablity between 1 nm and 450 nm.

En raison d’un désordre aléatoire à longue distance, un verre présente une symétrie d'inversion telle que la génération de seconde harmonique (GSH) est interdite. Cependant, par irradiation avec un laser femtoseconde (fs) très focalisé, il est possible de précipiter des cristaux optiquement non linéaires, et de rompre la symétrie d'inversion et donc d'induire une GSH. De plus, ceci peut être réalisé localement en trois dimensions. Pour la démonstration, on a appliqué, dans le système vitreux Li₂O-Nb₂O₅-SiO₂ le mode opératoire décrit ci-dessous qui permet la formation de cristaux de LiNbO₃, hautement optiquement non linéaire. La procédure est la suivante : 1) ajustement de la composition chimique du verre pour obtenir un verre suffisamment sensible au laser fs ; 2) contrôle des paramètres du laser (durée d'impulsion, fréquence de répétition des impulsions, vitesse de balayage du faisceau, énergie d'impulsion…) pour obtenir des nanocristaux avec répartition spatiale et taille correcte. En outre, la taille de la zone affectée doit être limitée ; 3) contrôle de l'orientation des nanocristaux. On montre qu'il est possible de satisfaire à cette condition, en contrôlant l'orientation de la polarisation du laser. Ceci a été montré par la méthode de rétrodiffusion d'électrons de diffraction (EBSD). En d'autres termes, ce processus peut être contrôlé directement avec la lumière. En outre, la spectroscopie par rayons X à dispersion d'énergie couplée à la microscopie à transmission électronique à balayage (STEM /EDS) et la microscopie électronique à transmission a révélé une microstructure orientable similaire à celle appelée nanoréseaux formée dans silice. L'originalité est que les nanocristaux optiques non linéaires texturées noyées dans un réseau de "murs" vitreux, sont alignés perpendiculairement à la direction de polarisation du laser. Il en résulte que la biréfringence et la propriété optique non linéaire peuvent être maîtrisées ensemble. Ceci est une percée dans ce travail de thèse. Ces résultats mettent en évidence des modifications spectaculaires de verre par rayonnement laser fs. Avec de nouvelles améliorations dans les techniques de fabrication, l'application de ce travail est de parvenir à réaliser un guide d'ondes biréfringent doubleur ou changeur de fréquences. / Due to random disorder, a glass exhibits inversion symmetry such that second harmonic generation (SHG) is forbidden. However, by irradiation with a tightly focused femtosecond (fs) laser, it is possible to induce nonlinear optical crystal precipitation, in order to break the inversion symmetry and thus to induce SHG. Moreover, this can be achieved locally in three dimensions. For demonstration, we applied the procedure described below in the glass system Li₂O-Nb₂O₅-SiO₂ that allows the formation of LiNbO₃ crystal, a highly non linear optical one. The procedure is thus the following: 1) adjustment of the glass chemical composition for obtaining a glass sensitive enough to fs laser. 2) control of the laser parameters (pulse duration, pulse repetition rate, speed of beam scanning, pulse energy…) for obtaining nanocrystals with correct space distribution and size. In addition, the size of the affected zone has to be limited. 3) control of the orientation of the nanocrystals. We show that it is possible to fulfill this condition by controlling the laser polarization orientation. This has been achieved by electron backscatter diffraction method (EBSD). In other words, this process can be controlled with light directly. In addition, energy dispersive X-ray spectroscopy coupled to scanning transmission electron microscopy (STEM/EDS) and transmission electron microscopy revealed an orientable microstructure similar to the one called nanogratings form in silica. The originality here is a textured nonlinear optical nanocrystals embedded in a network of “walls” made of vitreous phase, aligned perpendicular to the laser polarization direction. It results that birefringence and nonlinear optical property can be mastered in the same time. This is a highly valuable aspect of the work. These findings highlight spectacular modifications of glass by fs laser radiation. With further improvements in the fabrication techniques, the application of this work is to achieve SHG waveguide and birefringence-based devices.

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