The topic of this thesis is about experimental study of phenomena which are associated with light propagation in nonlinear dielectric media. In the first part of this work, we study experimentally the snake instability of the bright soliton stripe of the (2+1)-dimensional hyperbolic nonlinear Schrödinger equation. The instability is observed, through spectral measurements, on spatially extended femtosecond pulses propagating in a normally dispersive self-defocusing semiconductor planar waveguide. The second part of this thesis is about light propagation in nonlinear periodic media. We experimentally observe a stationary spatial gap (or Bragg) soliton in a periodic semiconductor planar waveguide. Based on the interference pattern of the soliton beam, we measure the power parameter of the soliton which is related to the position of the spatial spectrum in the linear band gap. <p><p><p>Cette thèse de doctorat a pour sujet l’étude expérimentale de phénomènes associés à la propagation de la lumière dans les milieux diélectriques non linéaires. La première partie porte sur la démonstration expérimentale de l’instabilité serpentine d’une bande solitonique dans un système décrit par une équation de Schrödinger non linéaire à (2+1)-dimensions. L’instabilité est observée sur base de mesures du spectre spatial ainsi que du profil spatio-fréquentiel d’une impulsion femtoseconde après propagation dans un guide plan semi-conducteur qui présente une dispersion normale et une non-linéarité défocalisante. Le second thème abordé concerne la propagation de la lumière dans les milieux non linéaires périodiques. Les expériences réalisées ont montré l’existence du soliton de Bragg spatial stationnaire sous forme de faisceaux se propageant dans des guides plans semi-conducteurs périodiquement gravés. Sur base du profil de la distribution modale en intensité du faisceau soliton, il a été possible de mesurer le paramètre de puissance du soliton de Bragg qui détermine la position du spectre spatial dans la bande interdite linéaire. <p> / Doctorat en sciences appliquées / info:eu-repo/semantics/nonPublished

This dissertation investigates two long standing issues in nonlinear optics: complete characterization of the ultrafast dynamics of simple molecules, and the potential of a two-photon laser using a bulk semiconductor gain medium. Within the Born-Oppenheimer approximation, nonlinear refraction in molecular liquids and gases can arise from both bound-electronic and nuclear origins. Knowledge of the magnitudes, temporal dynamics, polarization and spectral dependences of each of these mechanisms is important for many applications including filamentation, white-light continuum generation, all-optical switching, and nonlinear spectroscopy. In this work the nonlinear dynamics of molecules are investigated in both liquid and gas phase with the recently developed beam deflection technique which measures nonlinear refraction directly in the time domain. Thanks to the utility of the beam deflection technique we are able to completely determine the third-order response function of one of the most important molecular liquids in nonlinear optics, carbon disulfide. This allows the prediction of essentially any nonlinear refraction or two-photon absorption experiment on CS2. Measurements conducted on air (N2 and O2) and gaseous CS2 reveal coherent rotational revivals in the degree of alignment of the ensemble at a period that depends on its moment of inertia. This allows measurement of the rotational and centrifugal distortion constants of the isolated molecules. Additionally, the rotational contribution to the beam deflection measurement can be eliminated thanks to the particular polarization dependence of the mechanism. At a specific polarization, the dominant remaining contribution is due to the bound-electrons. Thus both the bound-electronic nonlinear refractive index of air, and second hyperpolarizability of isolated CS2 molecules, are measured directly. The later agrees well with liquid CS2 measurements, where local field effects are significant. The second major portion of this dissertation addresses the possibility of using bulk semiconductors as a two-photon gain medium. A two-photon laser has been a goal of nonlinear optics since shortly after the original laser*s development. In this case, two-photons are emitted from a single electronic transition rather than only one. This processes is known as two-photon gain (2PG). Semiconductors have large two-photon absorption coefficients, which are enhanced by ~2 orders of magnitude when using photons of very different energies, e.g., ћωa≈10ћωb. This enhancement should translate into large 2PG coefficients as well, given the inverse relationship between absorption and gain. Here, we experimentally demonstrate both degenerate and nondegenerate 2PG in optically excited bulk GaAs via pump-probe experiments. This constitutes, to my knowledge, the first report of nondegenerate two-photon gain. Competition between 2PG and competing processes, namely intervalence band and nondegenerate three-photon absorption (ND-3PA), in both cases are theoretically analyzed. Experimental measurements of ND-3PA agree with this analysis and show that it is enhanced much more than ND-2PG. It is found for both degenerate and nondegenerate photon pairs that the losses dominate the two-photon gain, preventing the possibility of a two-photon semiconductor laser.

The two-photon absorption (TPA) coefficient is measured in indium phosphide (InP) using femtosecond pulses to be 45cm/GW at 1.32μm. Nanosecond pulses are subsequently used to find the free-carrier refractive index cross-section, σ_r, and the free-carrier absorption coefficient, σ_fca. The quantity βσ_r is measured to be -113x10⁻²ºcm⁴/GW at 1.064μm and -84x10⁻²ºcm⁴/GW at 1.534μm. At 1.064μm, with β assumed to be 22cm/GW, the value suggested by theory, σ_r is -5.1x10⁻²ºcm³. Similarly, at 1.534μm, assuming β to be 20cm/GW gives a σ_r value of -4.1x10⁻²ºcm³. Due to refraction affecting the measurements of σ_fca, only an upper limit of 1x10⁻¹⁵cm² can be put on its value. The free-carrier experiments are repeated on two samples of cadmium mercury telluride (CMT) having bandgaps of 0.89eV and 0.82eV. For the first sample, β_σr is measured to be -148x10⁻²ºcm⁴/GW. Assuming β to be 89cm/GW gives a σ_r value of -1.7x10⁻²ºcm³ whilst σ_fca is found to be at most 3x10⁻¹⁵cm². Significant linear absorption occurs in the second sample which generates a large free-carrier population. It is shown that this significantly enhances the nonlinearities. Finally, the results of the work are tested by modelling a nonlinear transmission experiment, and the results found in this work give a closer fit to experimental results than the result of theory. Four-wave mixing (FWM) in a photonic crystal fibre is exploited to create a high output power optical parametric amplifier (OPA). To optimise the OPA conversion efficiency, the fibre length has to be increased to 150m, well beyond the walk-off distance between the pump and signal/idler. In this regime, the Raman process can take over from the FWM process and lead to supercontinuum generation. The OPA exhibits up to 40% conversion efficiency, with the idler (0.9μm) and the signal (1.3μm) having a combined output power of over 1.5W.

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We have conducted a detailed experimental and theoretical study of nonlinear absorption in semiconductors. Experimental measurements were made on a variety of materials at wavelengths of 1.06 and 0.53 microns using a picosecond Nd:YAG laser. Both two- and three-photon processes were investigated. Values of nonlinear absorption coefficients extracted from these measurements show excellent agreement with recent theory and scaling rules. Our theoretical investigation has been carried out for two-, three-,and n-photon absorption, for both continuous and pulsed sources. Expressions are obtained for the transmission of the sample in terms of the incident irradiance for each case. The physical interpretation of these results is discussed. We have also considered the effects of the photogenerated carriers on the measurements. Equations are developed that include linear absorption by these carriers. We have observed severe distortions on the transmitted beam, caused by changes in the refractive index of the material, due to the presence of these carriers. We present a model that accurately describes these effects in terms of the photogenerated carrier density. We have developed several novel techniques for monitoring nonlinear absorption. In particular, we have adapted the photoacoustic technique to the measurement of nonlinear absorption in semiconductors. We have also developed a technique employing irradiance modulation to greatly enhance the sensitivity to nonlinear processes and simultaneously discriminate against linear background signals. A related technique has been used to observe coherent mixing effects in semiconductors with cw, modelocked dye lasers.

The nonlinear refractive index (n2) of room temperature liquid CS2 in the wavelength range of 9 to 11 micrometers is measured. A line tunable hybrid C02 TEA laser and amplifier system is used for the experiments. In these measurements the well known photoacoustic method is utilized to observe the onset of whole beam self-focusing. The photoacoustic signal in a CS2 cell, much longer than the confocal parameter, is monitored. The departure of the acoustic signal from linear growth marks the critical power for the onset of nonlinearity. It is experimentally verified that the phenomenon is power dependent as expected from self-focusing theory. The value of n2 is then calculated from the theoretical model of self focusing. Measurements of the on-axis irradiance transmitted through the nonlinear material as well as the measurements of beam distortion are used to verify the validity of the photoacoustic method. In all the measurements the on-axis intensity was smaller than the calculated threshold intensity for stimulated Brillouin scattering. The back reflection was monitored to make sure that stimulated Brillouin scattering was not playing a role in the phenomenon.

Performance and reliability of solid state laser diodes in the IR region exceeds those in the visible and UV part of the light spectrum. Single frequency visible and UV laser diodes with higher than 500 mW power are not available commercially. However we successfully stabilized a multi-longitudinal mode IR laser to 860 mW single frequency. This means high efficiency harmonic generation using this laser can produce visible and UV laser light not available otherwise. In this study we examined three major leading nonlinear crystals: PPMgO:SLN, PPKTP and PPMgO:SLT to generate blue light by second harmonic generation. We achieved record high net conversion efficiencies 81.3% using PPMgO:SLT (~500 mW out), and 81.1% using PPKTP (~700 mW out). In both these cases an external resonance buildup cavity was used. We also studied a less complicated single pass waveguide configuration (guided waist size of ~ 5 um compared to ~60 um) to generate blue. With PPMgO:SLN we obtained net 40.4% and using PPKT net 6.8% (110mW and 10.1 mW respectively).

Les nanostructures métalliques ont la capacité de supporter des résonances de plasmons de surface localisés se caractérisant par une oscillation collective des électrons libres du métal. Ce phénomène, connu pour générer localement un champ électrique intense, peut notamment être exploité afin d'exalter les processus d'optique non-linéaire à l'échelle nanométrique. Au cours de cette thèse, nous nous sommes intéressés au processus de génération de second harmonique (SHG) de nanostructures en aluminium et en or. Tout d'abord, nous avons étudié l'origine du processus non-linéaire et mis en évidence le rôle important joué, dans l'or, par la contribution non-locale, issue des gradients de champ dans le volume de la nanostructure. Ensuite, nous avons montré, en associant un phénomène de double résonance et un accord des modes plasmoniques à l'excitation et à l'émission, qu'il est possible d'exalter fortement la réponse harmonique d'une nanoantenne compacte en aluminium. Dans l'optique d'obtenir une intensité non-linéaire encore plus importante, une stratégie est de coupler ces nanostructures à un nanocristal non-linéaire afin de bénéficier à la fois de la forte exaltation du champ générée par le métal et de la non-linéarité du cristal. Afin d'optimiser l'intensité harmonique générée par ces structures hybrides, disposer de nanocristaux possédant une forte non-linéarité intrinsèque est nécessaire. C'est pourquoi, au cours de cette thèse, nous avons mesuré la réponse harmonique de nanocristaux d'iodates de lantane isolés, afin d'estimer leur potentiel pour intégrer ce type de structure. De plus, un microscope optique en champ proche a été mis en place sur le dispositif expérimental permettant la manipulation de nanocristaux à proximité de structures métalliques. Cette thèse, en apportant de nouveaux éléments pour comprendre et optimiser le processus de SHG dans les nanostructures plasmoniques, offre de nouvelles perspectives pour confectionner des composants optiques efficaces pour la conversion de fréquence à l'échelle nanométrique. / Plasmonic nanostructures have the ability to support localised surface plasmon resonances characterized by a collective oscillation of the free electrons in metal. This phenomenon, know to generate an intense local field, can be used to enhance nonlinear optical processes at the nanoscale level. In this thesis, we have investigated the second harmonic generation (SHG) process in aluminum and gold nanostructures. First, we have studied the origin of this nonlinear process and highlighted the major role played, in gold, by the bulk nonlocal contribution, originating from the field gradients inside the nanostructure volume. Then, we pointed out, by achieving a double resonance regime associated with a plasmonic mode matching at the excitation and emission, the possibility to enhance significantly the harmonic response of compact aluminum nanoantennas. In order to increase even more the nonlinear intensity, an idea is to couple these nanostructures to a nonlinear nanocrystal to benficiate both from the field enhancement provided by the metallic nanoantenna and from the nonlinearity of the nanocrystal. To optimise the harmonic intensity generated by these hybrid structures, have nanocrystals with a strong intrinsic nonlinearity is required. To this end, we have measured the harmonic response of single latanide iodate nanocrystals, in order to evaluate their ability to integrate this type of structure. Moreover, we have implemented a near-field optical microscope used to manipulate nancorystals in the vincinity of metallic nanostructures. This thesis, by bringing new elements to understand and optimise the SHG process in plasmonic nanostructures, provides new perspectives to elaborate efficient optical components to frequency conversion at the nanoscale.

We investigate two medium-facilitated interactions between properties of light upon propagation through optical fiber. The first is interaction between the spin and intrinsic orbital angular momentum in a linear optical medium. This interaction gives rise to fine structure in the longitudinal momenta of fiber modes and manifests in rotational beating effects. We probe those beating effects experimentally in cutback experiments, where small segments are cut from the output of a fiber to probe the evolution of both output polarization and spatial orientation, and find agreement between theoretical predictions and measured behavior. The second is nonlinear optical interaction due to cross- and self-phase modulation between the complex-valued temporal amplitude profile of pump pulses and the amplitude profiles of generated signal and idler pulses in optical fiber photon-pair sources utilizing the four-wave mixing process named modulation instability. We develop a model including the effects of these nonlinear phase modulations (NPM) describing the time-domain wave function of the output biphoton in the low-gain regime. Assuming Gaussian temporal amplitude profiles for the pump pulse, we numerically simulate the structure of the biphoton wave function, in symmetric and asymmetric group velocity matching configurations. Comparing the overlap of the joint temporal amplitudes with and without NPM indicates how good of an approximation neglecting NPM is, and we investigate the effects of NPM on the Schmidt modes. We find that effects of NPM are small on temporally separable sources utilizing symmetric group velocity matching, but appreciably change the state of temporally entangled sources with the same group velocity matching scheme. For sources designed to produce entangled biphotons, our simulations suggest that NPM increases the Schmidt number, which may increase entanglement resource availability with utilization of a phase-sensitive detection scheme. We find that NPM effects on temporally separable sources designed with asymmetric group velocity matching produce non-negligible changes in the state structure. The purity is unaffected at perfect asymmetric group velocity matching, but if the pump is detuned from the correct wavelength, the purity degrades. The largest changes to the state due to NPM occur in long fibers with long pulse durations and low repetition rates.