Exziton-Polaritonen in Mikrokavitäten sind Quasi-Teilchen, die unter bestimmten physikalischen Konditionen kondensieren und damit in einen energetisch gleichen, gemeinsamen makroskopischen Quantenzustand (MQZ) übergehen können. Exziton-Polariton-Kondensate können mithilfe von akustischen Oberflächenwellen moduliert werden, um ihre Eigenschaften zu verändern. Dies ist insbesondere von großer Relevanz für zukünftige Anwendungen. In dieser Arbeit wurden die Struktur sowie die Dynamik der Exziton-Polariton-Kondensate in den durch die akustischen Oberflächenwellen erzeugten quadratischen Gittern untersucht. Es wurde dazu die Wellenfunktion der Exziton-Polariton-Kondensate im Rahmen der spektroskopischen und zeitaufgelösten Messungen im Orts- und Impulsraum abgebildet. Die MQZ wurden in einer optisch-parametrischen Oszillatorkonfiguration resonant angeregt. Die spektroskopischen Messungen zeigten, dass Exziton-Polariton-Kondensate in akustischen quadratischen Gittern aus unterschiedlichen MQZ, nämlich aus einem zwei-dimensionalen Gap-Soliton (2D GS) umgeben von mehreren ein-dimensionalen MQZ, und einem inkohärenten Strahlungshintergrund zusammengesetzt sind. Im Rahmen der zeitaufgelösten Experimente wurde die Dynamik der Wellenfunktion des 2D GS untersucht. Die zeitaufgelösten Ergebnisse zeigten, dass sowohl die Intensität der von dem 2D GS emittierten Photolumineszenz (PL) als auch die Kohärenzlänge des 2D GS zeitlich oszillieren. Die Intensität der PL und die Kohärenzlänge hängen von der Anregungsleistung, der Größe des Laserspots sowie von der relativen Position des akustischen Gitters und dem Laserspot ab. Im Ausblick dieser Arbeit wurde theoretisch die Anregung von Tamm-Plasmon/Exziton- Polaritonen (TPEP) sowie deren Modulation mithilfe von akustischen Oberflächenwellen diskutiert. TPEP entstehen durch die Superposition der in der Grenzschicht zwischen Mikrokavität und Metall angeregten Tamm-Plasmonen und den in der Mikrokavität erzeugten Exziton-Polaritonen. / Microcavity (MC) exciton-polaritons can form condensates, i.e. macroscopic quantum states (MQSs), as well under a periodic potential modulation. The modulation by a surface acoustic wave (SAW) provides a powerful tool for the formation of tunable lattices of MQSs in semiconductor MC. In this work, fundamental aspects of the structure and dynamics of exciton-polariton condensate in acoustic square lattices were investigated by probing its wavefunction in real- and momentum space using spectral- and time-resolved studies. The MQSs were resonantly excited in an optical parametric oscillator configuration. The tomographic study revealed that the exciton-polariton condensate structure self-organises in a concentric structure, which consists of a single, two-dimensional gap soliton (2D GS) surrounded by one-dimensional MQSs and an incoherent background. 2D GS size tends to saturate with increasing particle density. The experimental results are supported by a theoretical model based on the variational solution of the Gross-Pitaevskii equation. Time-resolved studies showed the evolution of the 2D GS wavefunction at the acoustic velocity. Interestingly, the photoluminescence (PL) intensity emitted by the 2D GS as well as its coherence length oscillate with time. The PL oscillation amplitude depends on the intensity and the size of the exciting laser spot, and increases considerably for excitation intensities close to the optical threshold power for the formation of the MQS. In the outlook, the formation of Tamm-Plasmon/Exciton-Polariton (TPEP) hybrid states and their modulation by SAWs was theoretically discussed. Here, the upper DBR is partly replaced by a thin metal layer placed on top of the MC. In this case, TPEP form by the superposition of Tamm plasmons at the metal-semiconductor interface and the exciton-polaritons in the MC.

Ce travail de thèse porte sur l'étude expérimentale de structures à plasmons Tamm actives, composées d'une couche d'argent déposée sur un miroir de Bragg semiconduc­ teur AlGaAs/GaAs contenant des puits quantiques InGaAs. Après une description des modes Tamm et de leurs propriétés planaires, nous nous sommes intéressés plus parti­ culièrement aux structures à plasmons Tamm confinés par un micro-disque de métal. Des mesures de photoluminescence ont permis de mettre en évidence un effet laser dans ces structures. Une étude approfondie a montré une évolution du seuil laser en fonction du diamètre du disque, résultant d'un compromis entre confinement et pertes. Dans un second temps, nous avons étudié la réponse optique de structures à plasmon Tamm asy­ métriques, où le plasmon Tamm est confiné par des micro-rectangles. Cette asymétrie lève la dégénérescence en énergie qui existe entre les deux modes linéairement polarisés de la structure. Ceci, associé à un fort désaccord spectral entre l'émission des puits et le plasmon Tamm, permet d'obtenir une émission laser linéairement polarisée . Enfin, nous présentons l'étude d'une structure à plasmon Tamm comportant un réseau permettant le couplage du plasmon Tamm au plasmon de surface de l'interface air/argent. Grâce à des mesures tirant parti de l'aspect propagatif des modes, nous avons mis en évidence un battement entre plasmon Tamm et plasmon de surface / This thesis focuses on the experimental study of actives Tamm plasmons structures, consisting in a layer of silver deposited on a AlGaAs/GaAs semiconductor Bragg mir­ ror which con.tains InGaAs quantum wells. After describing Tamm planar modes and their properties, we focused particularly on structures where Tamm plasmons are la­ terally confined by a metallic micro-disk. Photoluminescence measurements have been carried out in order to demonstrate lasing in these structures. A comprehensive study has shown a change in the lasing threshold with the diameter of the disk, resulting from a compromise between the confinement and the lasses. Secondly, we studied the optical response of asymmetric Tamm plasmon structures, where the Tamm plasmon is confined by micro-rectangles. This asymmetry lifts the degeneracy of energy between the two linearly polarized modes of the structure. Combined with a strong spectral de­ tuning between the quantum wells emission and the Tamm plasmon, this allows linearly polarized laser emission to set-up. Finally, we present the study of a Tamm plasmon structure comprising a gratting to couple the Tamm plasmon to the surface plasmon at the silver/air interface. Thanks to propagation measurements, we have highlighted the beating between Tamm plasmon and surface plasmon modes

We discuss approaches to increase the light outcoupling efficiency in organic microcavity (MC) lasers and organic light-emitting diodes (OLEDs). We find that the introduction of metals into the cavities leads to additional Tamm-plasmon polariton modes, while the corrugation of metal contacts, such as perforated m-size holes or a periodic array of metal stripes, leads to 2D confinement of the cavity modes, which in turn reduces the lasing threshold in MCs. Furthermore, we elucidate light loss mechanisms in OLEDs and reveal how external dielectric layers and periodic gratings can be used to enhance outcoupling from the OLED cavity.

An electrical driven organic solid state laser is a very challenging goal which is so far well beyond reach. As a step towards realization, we monolithically implemented an Organic Light Emitting Diode (OLED) into a dielectric, high quality microcavity (MC) consisting of two Distributed Bragg Reflectors (DBR). In order to account for an optimal optical operation, the OLED structure has to be adapted. Furthermore, we aim to excite the device not only electrically but optically as well. Different OLED structures with an emission layer consisting of Alq3:DCM (2 wt%) were investigated. The External Quantum Efficiencies (EQE) of this hybrid structures are in the range of 1-2 %, as expected for this material combination. Including metal layers into a MC is complicated and has a huge impact on the device performance. Using Transfer-Matrix-Algorithm (TMA) simulations, the best positions for the metal electrodes are determined. First, the electroluminescence (EL) of the adjusted OLED structure on top of a DBR is measured under nitrogen atmosphere. The modes showed quality factors of Q = 60. After the deposition of the top DBR, the EL is measured again and the quality factors increased up to Q = 600. Considering the two 25-nm-thick-silver contacts a Q-factor of 600 is very high. The realization of a suitable encapsulation method is important. Two approaches were successfully tested. The first method is based on the substitution of a DBR layer with a layer produced via Atomic Layer Deposition (ALD). The second method uses a 0.15-mm-thick cover glass glued on top of the DBR with a 0.23-µm-thick single-component glue layer. Due to the working encapsulation, it is possible to investigate the sample under ambient conditions.

Mémoire numérisé par la Direction des bibliothèques de l'Université de Montréal.

<p>The accurate description of ground and electronic excited states is an important and challenging topic in quantum chemistry. The pairing matrix fluctuation, as a counterpart of the density fluctuation, is applied to this topic. From the pairing matrix fluctuation, the exact electron correlation energy as well as two electron addition/removal energies can be extracted. Therefore, both ground state and excited states energies can be obtained and they are in principle exact with a complete knowledge of the pairing matrix fluctuation. In practice, considering the exact pairing matrix fluctuation is unknown, we adopt its simple approximation --- the particle-particle random phase approximation (pp-RPA) --- for ground and excited states calculations. The algorithms for accelerating the pp-RPA calculation, including spin separation, spin adaptation, as well as an iterative Davidson method, are developed. For ground states correlation descriptions, the results obtained from pp-RPA are usually comparable to and can be more accurate than those from traditional particle-hole random phase approximation (ph-RPA). For excited states, the pp-RPA is able to describe double, Rydberg, and charge transfer excitations, which are challenging for conventional time-dependent density functional theory (TDDFT). Although the pp-RPA intrinsically cannot describe those excitations excited from the orbitals below the highest occupied molecular orbital (HOMO), its performances on those single excitations that can be captured are comparable to TDDFT. The pp-RPA for excitation calculation is further applied to challenging diradical problems and is used to unveil the nature of the ground and electronic excited states of higher acenes. The pp-RPA and the corresponding Tamm-Dancoff approximation (pp-TDA) are also applied to conical intersections, an important concept in nonadiabatic dynamics. Their good description of the double-cone feature of conical intersections is in sharp contrast to the failure of TDDFT. All in all, the pairing matrix fluctuation opens up new channel of thinking for quantum chemistry, and the pp-RPA is a promising method in describing ground and electronic excited states.</p> / Dissertation

Organic microcavities comprising the host:guest emitter system Alq3:DCM offer an interesting playground to experimentally study the dispersion characteristics of laterally patterned microlasers due to the broad emission spectrum and large oscillator strength of the organic dye. By structuring of metallic or dielectric sublayers directly on top of the bottom mirror, we precisely manipulate the mode structure and in fluence the coherent emission properties of the device. Embedding silver layers into a microcavity leads to an interaction of the optical cavity-state in the organic layer and the neighboring metal which red-shifts the cavity resonance, creating a Tamm-plasmon-polariton state. A patterning of the metal can in turn be exploited to fabricate deep photonic wells of micron-size, efficiently confining light in lateral direction. In periodic arrays of silver wires, we create a Kronig-Penney-like optical potential in the cavity and in turn observe optical Bloch states spanning over several photonic wires. We modify the Kronig-Penney theory to analytically describe the full far-field emission dispersion of our cavities and show the emergence of either zero- , π-, or 2π- phase-locking in the system. By investigating periodic SiO2 patterns, we experimentally observe stimulated emission from the ground and different excited discrete states at room temperature and are able to directly control the laser emission from both extended and confined modes of the photonic wires at room-temperature.