No description available.

Surface plasmon-polaritons are optical surface waves formed through the interaction of photons with free electrons at the surface of metals. They offer interesting applications in a broad range of scientific fields such as physics, chemistry, biology, and material science. However, many of such applications face limitations imposed by the high propagation losses of these waves at visible and near-infrared wavelengths, which result mainly from power dissipation in the metal. In principle, the propagation losses of surface plasmon-polaritons can be compensated through optical amplification. The objective of this thesis is to provide deeper insights on the physics of surface plasmon-polariton amplification and spontaneous emission in surface plasmon-polariton amplifiers through theoretical and experimental vehicles applied (but not necessarily restricted) to a particular plasmonic mode termed long-range surface plasmon-polariton. On the theoretical side, the objective is approached by developing a realistic theoretical model to describe the small-signal amplification of surface plasmon-polaritons in planar structures incorporating dipolar gain media such as organic dye molecules, rare-earth ions, and quantum dots. This model takes into account the inhomogeneous gain distribution formed near the metal surface due to a non-uniform excitation of dipoles and due to a position-dependent excited-state dipole lifetime that results from near-field interactions between the excited dipoles and the metal. Also, a theoretical model to describe the amplified spontaneous emission of surface plasmon-polaritons supported by planar metallic structures is developed. This model takes into account the different energy decay channels into which an exited dipole located in the vicinity of the metal can relax. The validity of this model is confirmed through experimentation. On the experimental side, the objective is approached by providing a direct experimental demonstration of complete loss compensation in a plasmonic waveguide. The experiments are conducted using the long-range surface plasmon-polariton supported by a symmetric thin gold waveguide incorporating optically pumped organic dye molecules in solution as the gain medium. Also, an experimental study of spontaneous emission in a long-range surface plasmon-polariton amplifier is presented. It is shown that this amplifier benefits from a low spontaneous emission into the amplified mode, which leads to an optical amplifier with low noise characteristics. The experimental setup and techniques are explained in detail.

The work described in this thesis involves the measurements of the optical gain and amplified spontaneous emission (A.S.E) spectrum of Pb1-xSnxTe epilayers and the establishment of conditions under which optically pumped Pb1-xSnxTe laser using a CO2 laser as pump source can be produced. Pb1-xSnxTe epilayers have been grown by a hot wall epitaxy (HWE) technique on BaF2 single crystal substrates and the optical gain which can be produced in these layers has been measured by pumping the films transversely with a N2 laser. A model for optical gain and stimulated emission as a function of pump intensity has been developed which has permitted for the first time in these materials, a direct comparison between the magnitude of the gain pumping rate, and the optical gain generated. The measured optical gain is in very good agreement with the model predicted gain. Good fits to the measured stimulated emission spectra were also obtained from the model prediction. It is shown that the gain for a given pump wavelength has a drastic dependence on the material doping density. According to the model, CO2 laser optically pumped Pb1-xSnxTe laser can be readily achieved, provided that epilayer doping densities can be reduced to values of 1017 cm-3 or less. Nevertheless, doping densities even in nominally undoped layers are generally at least an order of magnitude too high. In some initial attempts to achieve lower doping densities, using a thermal annealing technique, doping densities as low as 2 x 10 17 cm-3 have been obtained and significant pump absorption was achieved at CO2 laser wavelength, as predicted by the model. / Thesis / Master of Engineering (ME)

In this work, we study the nonlinear propagation of light in liquid crystals (LCs) and the optical gain provided by LCs when they are polymer- or dye-doped.We will focus on nematic LCs, which are characterized by a mean orientation (also called director) of the elongated molecules and by a subsequent birefringence. After a general introduction on LCs, we focus on the nonlinear propagation of light in nematic LCs, and in particular the soliton-like propagation (nematicon). Indeed, if the light injected in the cell is intense enough, it can create a waveguide that counteracts the diffraction of the light. The light then propagates with an almost constant (or periodic) transverse profile.Our contribution to the subject starts with the numerical modeling of the thermal noise that characterizes the nematic LCs and the study of spatial instabilities of the soliton propagation caused by that noise. In Ch.3 we show that, by explicitly implementing the spatial correlation of the director in the LC thermal noise, it is possible to reproduce some of the features that characterize the LC response, such as the speckle generation or the fluctuating trajectory of the spatial optical soliton in LCs. Indeed, when the nematicon diameter is of the same order ofmagnitude as or smaller than the refractive index perturbations caused by the thermal noise, the nematicon starts to fluctuate in space. These fluctuations are not present when the noise is not correlated, indicating that the long-range interactions in LCs are crucial to explain the fluctuations. The model also allows us to introduce the propagation losses experienced by the nematicon without the use of an ad-hoc term. The simulations are in agreement with the experimental results. This method could also help the modeling of complex nonlinear phenomena in LCs that rely on noise, such as modulation instabilities or filamentation.Then, the optical gain is included in the LCs by dissolving photoluminescent polymers or dyes in it. In particular, we show that a particular polymer, the polyfuorene, when dissolved in nematic LCs, creates an intricate supramolecular pattern composed by homogeneous LC-rich regions surrounded by polymer-rich boundaries. The study of these structures through an ultra-fast spectroscopic technique (the pump-probe technique) and confocal microscopy reveals that the boundaries are composed by ordered and isolated chains of polymers. This particular morphology allows the observation of the optical gain from an oxidized unit of the polymeric chain (keto defects). This signal is usually covered by the absorption caused by the chain aggregation in solid state samples, while in LCs it is clearly visible. The optical gain from the keto defects appears also to be polarized orthogonal to the LC director, which is also the orientation of most of the boundaries. When a dye, one of the pyrromethenes, is dissolved in the LCs, the sample appears to be homogeneous. The optical gain from the dye ispolarized along the LC director and it shows an important spectral blue-shift (10 nm) passing from a polarization parallel to orthogonal to the LC director. The amplified spontaneous emission (ASE) shows the same shift when changing the direction of the sample excitation.When the ASE and the nematicon are generated in the same sample, it is possible to study the interaction between the two. In particular, the waveguide induced by the soliton can be used to guide another signal at another wavelength. We show that the nematicon can collect the ASE generated in the same device and guide it to the same fiber used to inject the nematicon in the LC cell. The extraction of the ASE from the device increases almost one order of magnitude when the soliton is present. However, due to the nematicon spatial fluctuations in LCs, an optimal nematicon power has to be found. Indeed, by increasing the soliton power, the light guiding is improved since the refractive index contrast of the nematicon-induced waveguide is increased. However, very high soliton powers have to be avoided, since the power-dependent soliton fluctuations prevent an optimal collection of the light. The nematicon is also found to increase the spectral purity and the polarization degree of the guided signal.Another LC system is studied, the chiral nematic LCs. In this system, the molecules are disposed following an helicoidal distribution. Due to their optical anisotropy and the periodic distribution, the system presents an optical band-gap. If the LC is also dye-doped, the combination of optical band-gap and gain generates laser emission. We are interested in a fast (sub-ms) reorientation of the helix, with the aim of studying the effect of this reorientation on the laser emission. The first step is the alignment of the LC helix (without the dye) with its axis parallel to the glass plates that constitute the cell, which is difficult to obtain with a high optical quality. For this reason, an innovative method is developed to align LCs through directional solvent evaporation. The solvent-induced method allows us to obtain particularly homogeneous textures, with a contrast ratio between the bright and the dark states that is a factor of 4 greater than that obtained with traditional methods. The LC samples based on solvent-induced alignment are then stabilized via two-photon photo-polymerization. This technique allows us to polymerize small regions of the device while the rest of the sample can be washed out in a solvent bath. When an achiral material is used to refill the device, it assumes a chiral alignment in the polymerized regions and an achiral nematic distribution in the rest. The first characterization of the laser emission is then presented in the last Chapter, with the aim of achieving sub-ms electrical tuning in future works.In this work a wide range of aspects have been investigated, leading to the realization of novel techniques for the fabrication of liquid crystal devices, the demonstration of novel phenomena for light amplification in liquid crystals and the experimental verification of new numerical modeling tools for light propagation in liquid crystals. The three key aspects of the work are nonlinear propagation, optical amplification and electrical response of different LC-based mixtures. Although the first few chapters deal with some of the aspects separately, in the last chapter these aspects are combined, revealing interesting new phenomena and pointing out a number of new aspects that could be part of future work. The results in this work have potential applications in fast tunable lasers, optical communication systems and lab-on-chip components. / Doctorat en Sciences de l'ingénieur et technologie / info:eu-repo/semantics/nonPublished

Free-electron lasers (FELs) are among the world's most intense artificial artificial sources of coherent light and are tunable to various wavelengths, including the X-ray spectrum. X-ray FELs (XFELs) are extremely useful for diffraction experiments to study molecules, materials, and quantum systems. A FEL consists of an electron accelerator and a structure of magnets called an undulator. The undulator has a periodic magnetic field, and when an electron beam passes through the undulator, the Lorentz force forces the electrons to oscillate and emit what is known asspontaneous undulator radiation. Initially, the undulator radiation is spontaneously emitted and incoherent. However, aAs the electrons interact with this initial spontaneous undulator radiation, they change their relative positions and form micro-bunches of electrons. These microbunches are shorter than the undulator radiation wavelength. Hence, the waves emitted by the electrons from the same microbunch arethey become in phase, meaning the radiation is now coherent with the radiation field, and the state of coherence develops. This process is known as self-amplified spontaneous emission (SASE). Due to the coherence, tThe radiation intensity grows exponentially along the undulator, forming several peaks in the radiation pulse known as SASE spikes. One technique for obtaining ultra-short laser pulses is to isolate single SASE spikes by controlling where, along the electron beam, the SASE spikes can grow. This growth limitation is archieved by modulating the electron energies, thus only allowing electrons at specific positions along the electron beam to radiate. In addition, to keep positive interference between undulator radiation from electrons with different energies, the energy modulation must be compensated with a gradient of the magnetic field amplitude of the undulator, so-called tapering. There are plans to implement this technique at one of the beamlines at the European X-ray FEL (EuXFEL) to generate attosecond X-ray pulses and study quantum systems. One goal of the design process is to choose design parameters for the electron beam's modulation amplitude and the undulator's tapering coefficient. These design parameters shall be chosen so that the XFEL will have as short pulse duration as possible while at the same time not getting too low peak power. This thesis aims to study the effect of electron energy modulation and undulator tapering on the SASE and how the modulation amplitude and the tapering coefficient affect the XFEL's peak power and pulse duration. A model was developed to simulate SASE with a modulated electron beam in a tapered undulator. With this model, a parameter scan gave the average peak power and pulse duration as functions of the modulation amplitude and the tapering coefficient. The parameter scan showed that the peak power and the pulse duration decrease as the modulation amplitude and the tapering coefficient increase. Therefore, a trade-off exists between high peak power and short pulse duration. It was possible to exclude sets of the parameters that gave too low peak power or long pulse duration. This study also found an optimum range for the tapering coefficient where the peak power had a local maximum without a significant increase in pulse duration. The physics behind this optimal tapering coefficient is also discussed in connection to the electrons' energy modulation.

No description available.

L'interaction matière-lumière dans des milieux opaques donne lieu à des phénomènes collectifs nécessitant le couplage d'équations atomiques et d'une équation de transport. Le piégeage de la lumière dans un système atomique multi-niveaux sera étudié expérimentalement dans une vapeur froide et théoriquement avec le couplage des paramètres atomiques à une équation de diffusion. Ensuite, du gain sera ajouté dans ce nuage d'atomes froids multi niveaux. Nous montrerons théoriquement qu'un seuil laser existe dans ce type de système combinant gain et diffusion et qu'expérimentalement le gain Raman associé à de la diffusion sur une raie résonante a permis l'observation d'un laser aléatoire à atomes froids. La validité de l'équation de diffusion nécessite une non redistribution en fréquence et donc des atomes suffisamment froids pour s'affranchir de l'effet Doppler. Finalement nous étudierons le transport dans une vapeur atomique chaude (20°C-180°C) opaque. L'effet Doppler invalide la loi de Beer-Lambert pour la longueur des pas des photons entre des diffusions qui suivent alors une statistique de Lévy. / The matter-light interaction in opaque media gives rise to collective effects which may be explained by the coupling between atomic equations and light transfer equation. The trapping of light in an opaque multi-levels atomic system will be studied experimentally in a cold vapour and theoritically. Then, this vapour will be in situation with gain and amplification of light occurs. We will show that a laser threshold exists with this kind of system. Experimentally, the mixing of Raman gain and multiple scattering on a resonant line allowed the abservation a cold-atom random laser. The validity of diffusion equation needs a non frequency shift and so the temperature of atoms should be sufficiently cold to avoid Doppler effect. Finally we study the transport of light in an opaque hot atomic vapour (20°C-180°C). The Doppler effect breaks the Beer-Lambert law for photons step size distribution which is then a Levy flight statictics.

Le développement du laser a ouvert la voix à l'exploration de nouveaux domaines scientifiques et industriels. Les impulsions laser à haute intensité sont un outil unique pour les études d'interaction lumière/matière et leurs applications. Mais elles sont générées par des systèmes laser reposant sur l'utilisation de milieux à gain en verre pompés par des lampes flashes et sont donc intrinsèquement limitées en termes de cadence et d'efficacité. Le développement, au cours de ces dernières années, des lasers semi-conducteurs a attiré l'attention sur une nouvelle classe de lasers, les « laser solides pompés par diodes » (DPSSL). Ils possèdent une grande efficacité et sont des candidats de choix pour les systèmes compacts à haute puissance moyenne requis pour des applications industrielles, mais aussi en tant que sources de pompe à haute puissance pour des lasers ultra-intenses. Les travaux décrits dans cette thèse s'inscrivent dans le cadre du système laser Lucia (1 kilowatt de puissance moyenne), actuellement en construction au «Laboratoire d'Utilisation des Intenses lasers» (LULI) à l'Ecole Polytechnique, France. La génération d'impulsions laser de durée sub-10 nanosecondes avec des énergies allant jusqu'à 100 joules et des taux de répétition de 10 hertz est principalement limitée par l'émission spontanée amplifiée (ASE) et les effets thermiques. L'étude de ces limitations est le thème central de ce travail. Leur impact est discuté dans le cadre d'un premier jalon énergétique fixé vers 10 joules. Le système laser mis au point est présenté en détails depuis l'oscillateur jusqu'à la fin de la chaine d'amplification. Une discussion complète de l'impact de l'ASE et des effets thermiques est complétée par des vérifications expérimentales. Les modèles de simulation informatique développés sont validés puis utilisés pour prédire les performances du système laser qui, lors d'une première activation, à atteint un niveau d'énergie de 7 joules en régime mono-coup et de 6,6 joules pour un taux de répétition de 2 hertz. Les limitations actuelles sont discutées ainsi que les approches envisagées pour des développements futurs.

The aim of this thesis is the preparation and characterization of model components for organic thin-film solid-state lasers. The theses focuses on comparing different methods of determining the threshold energy, which leads to an amplified spontaneous emission of the studied derivative diketo-pyrrolo-pyrrole. The theoretical part is devoted to a summary of knowledge on the interaction of light with matter and lasers with a focus on organic solid-state lasers. The practical part is focused on preparation of model components for organic solid-state lasers, modification of apparatus for their characterization, comparison of evaluation methods for determining the threshold energy and study of the effect of different conditions of components preparation.

V oblasti nových nízkomolekulárních organických materiálů patří deriváty difenyldiketopyrrolopyrrolu (DPP), používané dříve jako barviva a pigmenty, k objektům vysokého zájmu pro jejich potencionální aplikace v moderních technologiích. Studium jejich optických vlastností ve vztahu k jejich chemické struktuře umožní využití jejich vysokého potenciálu ve vývoji pokročilých inteligentních materiálů. Přehled chemických a fyzikálních vlastností DPP derivátů a zhodnocení současného stavu řešené problematiky jsou uvedeny v teoretické části této práce. Tři hlavní procesy studované v této práci jsou: klasická absorpce a emise, dvoufotonová absorpce (TPA) a zesílená spontánní emise (ASE). Výsledky budou diskutovány a shrnuty ve dvou částech: první zahrnuje první dvě výše zmíněné oblasti a druhá problematiku zesílené spontánní emise.