Diese Arbeit beschäftigt sich mit der Untersuchung der starken Kopplung und Laseremission in Strukturen, die ZnO, ZnCdO oder organische Moleküle als aktives Material enthalten. Die ZnCdO basierten Vielfachquantengräben erreichen ihre Laserschwelle durch optische Ruckkopplung an streuenden Luftlöchern. Diese Emitter nennt man random laser. Die Dynamik ihrer Emission unter quasi-stationären Bedingungen ist der hier gezeigte Fokus. Hoch reproduzierbare Anregungen werden verwendet um sowohl die Dynamik eines einzelnen Beschusses aber auch die Unterschiede verschiedener Anregungen zu untersuchen. Die experimentellen Daten werden durch numerische Simulation qualitativ reproduziert und mit Methoden der Netzwerktheorie interpretiert. Die verbreitetere optische Rückkopplung durch einen Resonator wird in der Untersuchung des Moleküls L4P und seiner Spiro-derivate benutzt. Zwei identische Braggspiegel umschließen die aktive Schicht aus L4P-SP2, das in eine Polymermatrix eingebettet ist, eine Dicke von 12 Mikrometer hat und in einer einzelnen Mode lasert (schwache Kopplung). Durch Verringerung der aktiven Schicht auf die Hälfte der Resonanzwellenlänge wird das System in den Bereich der starken Kopplung gebracht. Eine Rabi-Aufspaltung von 90 meV wird zu beiden vibronischen Resonanzen beobachtet. Die energetische Position in Resonanz zu ZnO macht dieses Molekül zu einem guten Kandidaten für die Fertigung einer hybriden Mikrokavität im Bereich der starken Kopplung. Dies wurde in einer teilweise epitaktisch gewachsenen Mikrokavität angewandt, die aus einem ZnMgO basierten Braggspiegel und sechs Quantengräben besteht. Darauf folgt eine aufgeschleuderte Schicht von L4P in der Polymermatrix. Der Resonator wird mit einem dielektrischen Spiegel fertiggestellt. Tieftemperatur Reflektion zeigt eine deutlichen ausweichen und eine gleichverteilte Mischung der drei Resonanz im mittleren Polaritonzweig. / This thesis presents the investigation of strong coupling and lasing in structures using ZnO, ZnCdO or organic molecules as active material. The ZnCdO based multi quantum well structures reach the lasing threshold by using scattering at air holes as the optical feedback. Such emitters are called random lasers. The dynamics of their emission under quasi-stationary condition is the point of interest presented. Highly reproducible excitations are used to investigate the single shot dynamics and their shot to shot differences. The experimental data is qualitatively reproduced by numerical simulation and interpreted by means of network theory. The more common optical feedback by a cavity is applied in the investigation of the molecule L4P and its spiro-derivatives. Using two identical SiO2/ZrO2 based Bragg reflectors surrounding an active layer of L4P-SP2 in a polymer matrix of approximately 12 microns thickness reached single mode lasing (weak coupling). Reducing the active layer thickness to half the resonance wavelength pushes the system into the strong coupling regime. Angular resolved reflectivity shows the anticrossing of the tuned cavity resonance to two vibronic transitions of the molecule. The Rabi-splitting to both vibronic resonances reaches around 90 meV. The energetic position in resonance to ZnO makes this molecule a promising candidate for a hybrid inorganic/organic microcavity in the strong coupling regime. This is used in a partially epitaxially grown microcavity composed of a ZnMgO based Bragg reflector (alternating layers of different Mg content) and six quantum wells. This is followed by a spincoated layer of L4P in a polymer matrix. The cavity is finished by a dielectric mirror. Low temperature reflectivity shows a clear anticrossing reaching an equal mixing of all resonances for the middle branch.

O interesse na pesquisa de Lasers randômicos, meios dispersivos com alto ganho, tem crescido nos últimos anos em virtude das novas possibilidades advindas ao se trabalhar com estes sistemas, como emissões em bandas com baixo ganho, bicromaticidade, localização da luz em meios difusos e sistemas ópticos mais compactos. Nesse trabalho serão discutidos temas como espalhamento da luz por partículas, intensidade de retroespalhamento, ganho em meios desordenados e as transições energéticas do neodímio, correlacionando as emissões características obtidas nos experimentos com a teoria. Quanto aos resultados será apresentado a primeira observação de laser randômico com nanopó de Nd:YVO4 através de análise do comportamento da emissão espectral e temporal oriunda da transição 4F3/24I11/2 (1064 nm). Os resultados apresentam outra forma de analisar a cinética temporal da emissão de laser randômico, permitindo uma separação da fração de emissão estimulada e espontânea e comparação desse resultado com o estreitamento sutil da largura de linha, típico de lasers randômicos. As conversões ascendentes e saturação de ETU (conversão ascendente por transferência de energia) serão analisadas na mesma amostra, sendo todos os ajustes provenientes da literatura e de fundamental interesse, principalmente por se tratarem de um mecanismo de perda em lasers operando na região do infravermelho. Por fim, a emissão característica será avaliada pela técnica CBS (retroespalhamento coerente) para determinação da coerência do laser emitido e localização da luz neste meio difuso, com os resultados comparados aos da simulação. / In the past few years, the interest in random lasers, which refer to lasing in disordered media where strong multiple scattering plays a constructive role instead of being only a loss factor, have received considerable attention due to its unique properties and its potential applications, such as emission at new, extremely low gain lines, simultaneous emission of several very different wavelengths at the same time, strong light localization and miniaturization. Single and multiple particle light scattering, backscattering intensity, light diffusion with gain and the energy level diagram of Neodymium will be presented in this current work, alongside with a parallel from the typical emission lines obtained experimentally with theory. The demonstration of random laser action in Nd:YVO4 nanopowder, by analyzing the spectral and temporal behavior from the 4F3/24I11/2 (1064 nm) transition is presented. A method that analyzes the decay kinetics after long-pulse excitation is used to determine the laser characteristics, allowing measuring the fractional contribution of spontaneous and stimulated emission in the samples backscattering cone, with is in agreement to the smoothing linewidth narrowing as a function of pump power typical from random lasers. Also the visible emission along a method to determine quantitatively the ETU (energy-transfer upconversion) rate is presented, which is particularly interesting, as is a mechanism that introduces a loss channel for devices emitting in the infrared region. At last, the coherent laser emission and light localization will be evaluated by using the CBS (coherent backscattering) technique in this diffusive media, in which the results are compared with simulation.

Dans cette thèse, nous nous intéressons aux propriétés des fluctuations de la lumière diffusée par un nuage d'atomes froids, que ce soit les variations temporelles de l'intensité ou les fluctuations spectrales du champ électrique dans le régime de diffusion simple ou multiple de la lumière. Bien que notre analyse soit réalisée sur un système passif, l'ajout de gain dans le système peut conduire à l'obtention d'un laser aléatoire dont l'étude des corrélations temporelles de l'intensité émise peut permettre une étude détaillée de ses propriétés de cohérence.La première étape de cette caractérisation est l'étude du bruit de fréquence de lasers conventionnels. La mesure est réalisée grâce à un discriminateur de fréquence, pouvant être une cavité Fabry-Pérot ou une transition atomique, utilisé pour convertir le bruit de fréquence en bruit d'intensité mesuré. Un modèle simple est présenté montrant que, alors que les résultats obtenus pour la cavité ou la transition atomique soient identiques à faibles fréquences de Fourier, de nouvelles structures apparaissent à hautes fréquences, permettant de réaliser de la spectroscopie de bruit en analysant les fluctuations de la lumière transmise.Les propriétés de cohérence peuvent aussi être étudiées grâce à la fonction de corrélation g(2) de l'intensité, offrant un accès à la statistique des photons de la lumière émise. Nous mesurons cette fonction dans un milieu passif en expansion balistique en contrôlant finement le régime de diffusion de la lumière. Nous analysons en détails l'évolution du contraste, la perte de cohérence ainsi que le changement de forme de g(2) dans le régime de diffusion multiple. Ces résultats sont combinés à des études numériques et analytiques pour mettre en évidence le rôle de la diffusion multiple dans les changements de la fonction g(2). Cette mesure est la première réalisation expérimentale de spectroscopie des ondes diffuses sur un nuage d'atomes froids en mouvement balistique.La caractérisation de la cohérence temporelle d'un laser aléatoire passe par l'étude de la fonction g(2) sur un milieu actif sous le seuil d'émission. Nous implémentons alors un schéma de gain Raman hyperfin, combinant efficacement gain et diffusion. Nous présentons les premiers tests de la quantification du gain dans le nuage par spectroscopie pompe-sonde, montrant l'apparition d'une fenêtre de transparence électromagnétiquement induite. Enfin, par une méthode hérérodyne, nous sommes en mesure d'accéder au spectre optique de la lumière diffusée en présence de gain. / In this thesis, we are interested in studying the properties of the fluctuations of the light scattered by a cloud of cold atoms, namely temporal fluctuations of the intensity or spectral fluctuations of the electric field in the single or multiple scattering of light. Although our analysis is focused on a passive medium, gain can be added in the system leading to a random laser whose the study of the temporal correlations of the emitted intensity allows to better characterize its coherence properties.The first step towards this characterization is the study of the frequency noise power spectral density of conventional lasers. This measurement is made using a frequency discriminator, being a Fabry-Pérot cavity or an atomic transition, used to convert frequency noise into measurable intensity noise. A simple model is developed showing that, while results obtained with the Fabry-Perot cavity and the atomic transition are the same at low Fourier-frequency, new features appear at high Fourier-frequency showing the influence of the atoms in the noise conversion, allowing to perform spectroscopic measurements by analyzing the intensity fluctuations of the transmitted light.Coherence properties can also be studied with the correlation function g(2) of the intensity, giving access to the photon statistics of the emitted light. We measure this function in a passive medium ballistically expanding while controlling the regime of scattering of light. We analyze in detail the evolution of contrast, the loss of coherence and the change of shape in the multiple scattering regime. Those results are combined with numerical and analytical studies showing the role of multiple scattering in the changes of the g(2)-function. This measurement is the first experimental demonstration of diffusing wave spectroscopy on cold atoms in ballistic motion.The characterization of the temporal coherence of a random laser requires the study of the g(2)-function in an active medium below threshold. We implement a scheme based on hyperfine Raman gain, combining effectively gain and scattering. We present our first results to quantify the amount of gain in the cloud with pump-probe spectroscopy, showing the appearance of an electromagnetically induced transparency window. Finally, based on a heterodyne method, we are able to access the optical spectrum of the scattered light in presence of gain.

[pt] Materiais nanoestruturados tem um espaço proeminente nos avanços tecnológicos devido a suas propriedades físicas e químicas que podem ser bem diferentes das encontradas no mesmo material em forma de bulk. Na primeira parte desta tese foram investigados, como centros espalhadores em laser aleatório (RL) materiais nanoestruturados naturais, como exemplo disso são o quartzito e a celulose. Nesse contexto, usamos celulose e o quartzito como centros espalhadores de lasers aleatórios, em suspensão com etileno glicol, com o intuito de caracterizar esses sistemas como lasers aleatórios, definindo-se o limiar laser e a variação da largura a meia altura do espectro de emissão laser. São apresentadas também outras configurações do laser aleatório como o filme espesso de celulose e onda guiada com suspensão de quartzito. Uma outra área de pesquisa com grande impulso, após a descoberta do grafeno, é aquela associada aos materiais 2D, tais como os Dicalcogenetos de Metais de Transição (TMDs). Na segunda parte desta tese está relacionada com a caracterização de propriedades ópticas não lineares (ONL) que tem uma enorme importância para aplicações de materiais 2D em dispositivos optoeletrônicos e em nanofotônica. Já na segunda parte dessa tese foram caracterizadas as propriedades de ONL térmica e eletrônica de materiais do tipo TMDs, para a determinação dos valores do índice de refração não linear e o coeficiente de absorção não linear desses materiais, usando a técnica de varredura Z (Z-Scan). / [en] Nanostructured materials have a prominent place in technological advances due to their physical and chemical properties that can be quite different from those found in the same material in bulk form. In the first part of this thesis, random laser scattering centers (RL) were investigated. natural nanostructured materials such as quartzite and cellulose. In this context, we used cellulose and quartzite as scattering centers for random lasers, suspended with ethylene glycol, to characterize these systems defining the laser threshold and full width half maximum (FWHM) of these random lasers. Other random laser configurations are also presented, such as thick cellulose film and guided wave with quartzite suspension. Another area of research with great impetus, after the discovery of graphene, is that associated with 2D materials, such as Transition Metal Dichalcogenides (TMDs). The second part of this thesis is related to the characterization of nonlinear optical properties (NLO) which is of enormous importance for applications of 2D materials in optoelectronic devices and in nanophotonics. In the second part of this thesis, the thermal and electronic NLO properties of TMD-type materials were characterized, to determine the values of the nonlinear refractive index and the nonlinear absorption coefficient of these materials, using the Z- scan technique.

Im Rahmen dieser Arbeit wurden die optischen Eigenschaften von auf ZnO-basierenden Heterostrukturen untersucht. Besonderes Augenmerk lag hierbei auf ihrer Eignung als aktives Material in Laserdioden für den ultravioletten und sichtbaren Spektralbereich. Es wurde gezeigt, dass ZnO und seine ternären Mischkristalle ZnCdO und ZnMgO erstaunlich vielfältige Anwendungen ermöglichen. Mit diesem Materialsystem lässt sich sowohl ein sehr großer Spektralbereich für Lasertätigkeit abdecken als auch eine Vielzahl von Laseranordnungen realisieren. Im Detail wurde demonstriert, dass sich die Lasertätigkeit von ZnCdO/ZnO Quantengraben-Strukturen vom violetten bis in den grünen Spektralbereich verschieben lässt. Obwohl diese Strukturen starke interne elektrische Felder aufweisen, konnte optisch gepumpte Lasertätigkeit bei Zimmertemperatur bis zu einer Wellenlänge von 510 nm gezeigt werden. Die für die Lasertätigkeit nötige optische Rückkopplung wird durch makroskopische Defekte der Probe verursacht und die Proben fungieren somit als Zufallslaser. Die Herstellung von Mikroresonatoren ermöglichte die Untersuchung des Zusammenspiels von Fabry-Perot- und Zufalls-Rückkopplung. Die experimentellen und theoretischen Ergebnisse zeigen, dass der Schwellengewinn eines Zufallslasers in der Regel größer ist als der des Fabry-Perot-Lasers. Des Weiteren wurde gezeigt, dass hoch reflektierende Braggreflektoren für den ultravioletten und blau/grünen Spektralbereich aus ZnO- und ZnMgO-Schichten hergestellt werden können. Ferner wurden die teils unbekannten Brechungsindexverläufe der verwendeten ternären Materialen erarbeitet und Mikrokavitäten mit ZnO/ZnMgO Quantengraben Strukturen als aktive Schichten realisiert. An diesen Kavitäten konnte bei Temperaturen bis zu 150 K starke Kopplung zwischen Exzitonen und Photonen nachgewiesen werden. Bei Zimmertemperatur konnte vertikal-emittierende Lasertätigkeit im nahen ultravioletten Spektralbereich demonstriert werden. / In the framework of this thesis, the optical properties of ZnO-based heterostructures fabricated by molecular beam epitaxy have been investigated, particularly with regard to their suitability for semiconductor laser devices operating in the ultraviolet and visible spectral range. It turned out that ZnO and its ternary alloys ZnMgO and ZnCdO are extremely versatile. They allow to tune the laser emission in a wide spectral range as well as to realize various laser geometries. In detail, it was shown that the laser emission of ZnCdO/ZnO multiple quantum wells can cover a spectral range from violet to green wavelengths. Although these structures suffer from large built-in electric fields, room temperature laser action under optical pumping was demonstrated up to a wavelength of 510. The optical feedback for lasing is provided by growth imperfections on a macroscopic length scale turning these structures into random lasers. The fabrication of micro-resonators allowed to study the interplay between random and Fabry-Perot feedback. The experimental and theoretical analysis shows that random feedback generally requires a larger gain than under Fabry-Perot feedback. Further, this work demonstrates that ZnO- and ZnMgO-layers can be used to fabricate highly reflective distributed Bragg reflectors for applications in the ultraviolet and blue/green spectral range. The partly unknown dispersion curves of the index of refraction of the employed ternary alloys have been elaborated. This enabled the realization of all monolithic microcavities with ZnO/ZnMgO quantum wells as active zone. For temperatures below 150 K strong exciton-photon coupling is observed in such microcavities. At room temperature, vertical cavity surface emitting laser action in the near UV spectral range is demonstrated for appropriately designed microcavities.