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Study of Transition Metal Dichalcogenides Via Linear and Non-Linear SpectroscopyStevens, Christopher E. 02 July 2019 (has links)
Beginning with the discovery of graphene, two-dimensional materials have amassed a strong interest. Like graphene, transition metal dichalcogenides (TMDs) can be coaxed into atomically thin sheets which have some impressive properties. Unlike graphene, TMDs also has a change in their electronic band structure causing an indirect band gap to a direct gap transition in its monolayer form. Additionally, these materials lose their inversion symmetry as a monolayer. These unique properties make TMDs a strong candidate for being used in optoelectronic and valleytronic devices. In order for these devices to be successful, the optical properties of TMDs must be thoroughly understood. Due to this class of material's strong Coulomb interaction, the optical properties are dominated by excitons, a quasiparticle made up of an electron-hole pair. Therefore, the success of these devices relies, in part, on understanding and manipulating excitons. One key parameter of excitons is their dephasing rate which characterizes the lifetime of the coherent superposition of two states (i.e. how the coherence decays which is caused by excitons interacting with their environment). In this work, two optical properties are investigated: (1) How the linear absorption of the TMDs A-exciton peak varies as the material increases in thickness. By looking at how the absorption varies by sample thickness, the interaction between emitters can be understood. Experimental results for the diamagnetic shift are presented which are used to determine the lateral excitonic size. Through theoretical calculations, based on the semiconductor Maxwell-Bloch equations, additional insight into the radiative coupling of the systems are obtained. (2) How the coherence prole of the exciton changes in the presence of an external magnetic eld and specic valley excitation. By varying the polarization scheme in the four wave mixing measurement, specic valley excitation can be selected, allowing for insight into the dephasing mechanisms. By applying an external magnetic eld, the energy levels of the electron and hole can be discretized and the corresponding eects on the system's coherence seen. In conjunction with time-dependent density function theory calculations and the experimental results, a deeper understanding of exciton dynamics and multi-exciton complexes was obtained. Finally, a new system is proposed in which complex spectroscopic techniques can be performed on micron sized samples as well as devices in the presence of an external magnetic eld at cryogen temperatures. This system will allow for the investigation of the optical properties of stacked monolayers (heterostructures) as well as devices.
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Super- et sous-radiance dans un nuage dilué d'atomes froids / Super- and subradiance in a dilute cloud of cold atomsOliveira de Araujo, Michelle 11 December 2018 (has links)
Le problème de l'interaction de N atomes avec un faisceau laser et les modes du vide peut donner lieu à de nombreux phénomènes intéressants concernant l’émission spontanée de la lumière et sa propagation dans l’échantillon. Les effets coopératifs, par exemple, tels que la super- et la sous-radiance, sont des effets liés à la cohérence créée entre les atomes lorsqu'un photon est émis spontanément par un seul atome excité. La super-radiance peut être définie comme le renforcement de l'émission spontanée due à une interférence constructive de la lumière diffusée. Son homologue, la sous-radiance, est le piégeage d'une partie de la lumière restante en raison d'interférences destructives. Dans les atomes froids, certains travaux théoriques antérieurs prédisent et caractérisent ces deux effets coopératifs dans un nuage atomique large et diluée, dans le régime des faibles intensités et à grands désaccords du laser incident. Le modèle théorique est un modèle de dipôles couplés pour atomes à deux niveaux pilotés par un champ de faible intensité et dans l'approche scalaire. L'expérience consiste à mesurer les taux de d’décroissance super- et sous-radiants à partir de l’intensité temporelle émise après la coupure du laser incident en régime stationnaire. Notre schéma expérimental consiste en un piège magneto-optique d’atomes de rubidium 87 à grandes épaisseurs optiques à résonance. Un faisceau sonde excite les atomes proches de la raie D2. L’intensité émise est détectée par un détecteur de photons uniques dépourvu d’afterpulsing et une procédure d’étalonnage nous permet de déterminer l’épaisseur optique résonante du nuage et sa température. Dans ce travail, nous rapportons l’observation expérimentale de la super- et sous-radiance dans un grand nuage d’atomes froids. Pour la sous-radiance, le résultat principal est l’évolution linéaire du temps caractéristique avec l’épaisseur optique résonante du nuage et son indépendance du désaccord. Pour la super-radiance, on observe la super-radiance en dehors de la direction vers l’avant. Nous vérifions la validité de nos interprétations avec les prédictions du modèle de dipôles couplés. Finalement, nous discutons l’interaction entre la sous-radiance et le piégeage de radiation, ainsi que des prévisions théoriques concernant : la configuration d’un nuage phasé, pour contrôler l’émission de l’amplitude sousradiante ; et les effets de température, où la sous-radiance s’avère robuste dans une large gamme de températures. / The problem of the interaction of N atoms with a laser beam and vacuum modes can give rise to many interesting phenomena concerning the spontaneous emission of light and its propagation in the medium. The cooperative effects, for example, such as superadiance and subradiance, are effects related to the coherence created between the atoms when a photon is emitted spontaneously by a single excited atom. Superradiance can be defined as the enhancement of the spontaneous emission due to constructive interference of the scattered light. Its counterpart, subradiance, is the trapping of some remaining light due to destructive interference. In cold atoms, some previous theoretical works predict and characterize these two cooperative effects in a large and diluted atomic cloud, in the regime of low intensities and large detunings of the incident laser. The theoretical model is a coupled-dipole model for two-level atoms driven by a low-intensity field and in the scalar approach. The experiment consists in measuring the super- and subradiant decay rates from the temporal emitted intensity after the switch off of the incident laser in the steady state. Our experimental setup consists in a magneto-optical trap of rubidium 87 atoms at large resonant optical thicknesses. A probe beam excites the atoms close to the D2 line. The intensity emitted is detected by a single photon detector with no afterpulsing and a calibration procedure allows us to determine the resonant optical thickness of the cloud and its temperature. In this work, we report the experimental observation of super- and subradiance in a large cloud of cold atoms. For subradiance, the main result is the linear evolution of the characteristic time with the resonant optical thickness of the cloud and its independence of the detuning. For superradiance, we observe superradiance out of the forward direction. We verify the validity of our interpretations with the predictions of the coupled-dipole model. Finally, we discuss the interplay of subradiance and radiation trapping, as well as theoretical predictions for: a setup of a phased cloud, to control the subradiant amplitude emission; and temperature effects, where subradiance is shown to be robust in a large range of temperatures.
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