Nonpolar ZnO/ZnMgO-based optical microcavities have been grown on (10-10) m-plane ZnO substrates by plasma-assisted molecular beam epitaxy. Reflectivity measurements indicate an exponential increase of the cavity quality factor with the number of layers in the distributed Bragg reflectors. Most importantly, microreflectivity spectra recorded with a spot size in the order of 2 lm show a negligible photonic disorder (well below 1 meV), leading to local quality factors equivalent to those obtained by macroreflectivity. The anisotropic character of the nonpolar heterostructures manifests itself both in the surface features, elongated parallel to the in-plane c direction, and in the optical spectra, with two cavity modes being observed at different energies for orthogonal polarizations.

We report on room temperature phonon-assisted whispering gallery mode (WGM) lasing in ZnO microwires. For WGM laser action on the basis of the low gain phonon scattering process high quality resonators with sharp corners and smooth facets are prerequisite. Above the excitation threshold power PTh of typically 100 kW/cm2, the recombination of free excitons under emission of two longitudinal optical phonons provides sufficient gain to overcome all losses in the microresonator and to result in laser oscillation. This threshold behavior is accompanied by a distinct change of the far and near field emission patterns, revealing the WGM related nature of the lasing modes. The spectral evolution as well as the characteristic behavior of the integrated photoluminescence intensity versus the excitation power unambiguously proves laser operation. Polarization-resolved measurements show that the laser emission is linear polarized perpendicular to the microwire axis (TE).

The ultrafast carrier dynamics of epitaxial ZnO and BaTiO3 thin films after intense excitation at 3.10 eV and 4.66 eV photon energy has been studied by femtosecond absorption spectroscopy. Modelling the transient transmission changes on the basis of spectroscopic ellipsometry data and pertinent equilibrium model dielectric functions extended by additional terms for the effects at high carrier density (P-band luminescence and stimulated emission from electron-hole-plasma), a self-consistent parameterized description was obtained for both materials. Excited carrier lifetimes in the range of ≈2 to ≈60 ps and long-lived thermal effects after several hundred ps have been identified in both materials. These findings form a reliable basis to quantitatively describe future femtosecond studies on ZnO/BaTiO3 heterolayer systems.

Within this thesis, photo-induced mechanisms of the light-matter interaction are investigated in tailored and photofunctional materials that differ significantly in their optical and structural properties. The individual coupling mechanisms in congruently melted, nominally undoped or iron doped lithium niobate crystals as well as in structurally disordered photoswitchable molecules embedded into a solid state polymer are examined in particular by the principle of holographic grating recording and transient absorption spectroscopy which provide new insight into a variety of material response properties. In case of photoswitchable ruthenium sulfoxide compounds, the underlying mechanism can be unambiguously assigned to a photochromic material response evoked by a photochemical reaction, i.e., a non-instantaneous, local ligand isomerisation. Comparable results are obtained for iron-doped, oxidized lithium niobate where holographic grating recording is related to the photophysical generation of transient excitonic states whose photochromic properties are characterized by targeted ns-pump, supercontinuum probe spectroscopy. In the event of nominally undoped lithium niobate, the holographic amplification of two sub-picosecond pulses is attached to the phenomenon of two-beam coupling on a self-induced dynamic grating. By correlating the individually obtained mechanisms of the light-matter interaction and the light-induced material response, generally accepted conclusions on a microscopic level can be achieved. A major influence of the internal structure and orientation of the excited states, i.e., an appropriate threedimensional structural arrangement, is deduced as a prerequisite for the formation of light-induced, macroscopic refractive index changes while absorption and microscopic refractive index alterations linked via the Kramers-Kronig relation are unaffected. In systems featuring a random distribution of excited states, an orientational order might be achieved as a consequence of linear polarized light, i.e., by polarization structuring. Moreover, if the photorefractive effect can be ruled out, the material response in lithium niobate can be solely assigned to a local alteration of the transient electronic states, i.e., to the photochromic properties of polarons and/or excitonic states, which is in particular comparable to the linkage isomerism of molecular photoswitchable molecules. In addition, the influence of structural parameters on the light-matter/surface interaction is studied on the μm-scale by analyzing the diffraction phenomenon arising from a relief grating. A considerable impact on the surface grating assisted coupling is determined by the transition from cw-lasers to ultrashort laser pulses which enables interference quenching. However, this phenomenon is of no consequence in case of selfinduced holographic gratings.

No description available.

<p>Cuprous oxide (Cu₂O) has recently been proposed as a promising solid-state host for ex-<br> citonic Rydberg states with large principal quantum numbers (n) whose exaggerated wave-<br> function sizes (∝ n²) facilitate gigantic, resonant dipole-dipole (∝ n⁴) and van der Waals<br> (∝ n¹¹) interactions, making them an ideal basis for solid-state Rydberg physics and quan-<br> tum technology. Synthetic, thin-film Cu₂O samples are of particular interest because they<br> can be made defect-free via carefully controlled fabrication and are, in principle, suitable<br> for the observation of extreme single-photon nonlinearities caused by Rydberg blockade. In<br> this work, we present the development of a spectroscopy experiment for characterizing the<br> behavior of Rydberg excitons and use it to study a synthetic thin film of Cu₂O grown on a<br> transparent substrate. We present evidence for the presence of states up to n = 8 and conduct<br> the first temperature-dependent study of Rydberg excitons in a thin film. We also propose<br> a technique for studying Rydberg-Rydberg interactions via the creation of high exciton den-<br> sities and establish a set of rate equations for modeling the processes by which excitons are<br> created, interact with each other, and decay. Finally, we conclude with a discussion of the<br> project’s outlook, as well as what future work will be undertaken to study the interactions<br> between Rydberg excitons and utilize them in scalable, integrable, Rydberg-based quantum<br> devices.<br> </p>

In my thesis I will discuss some aspects of collective dynamics of excitons and exciton-polaritons in nanoscale heterostructures. In the first Chapter I will make a brief introduction to the modern semiconductor physics and willdescribe the general elements and notions which will be used further. Other four chapters would be devoted to four works in which I participated, notably, in Chapter 2 I will speak about the coherent interactions between phonons and exciton orexciton-polariton condensates, in Chapter 3 I will discuss the quantum dots lasing and its amplification by an acoustic pulse. Chapter 4 and 5 will be devoted respectively to the polariton multistability and to the condensates of indirect excitons.

La décohérence dans les solides est un problème majeur vers la réalisation d'un processeur quantique basé sur l'utilisation de boîtes quantiques (BQs) semiconductrices comme qubits optiquement actifs. Mesurer et contrôler la cohérence optique de tels qubits s'avère donc primordial, tant d'un point de vue technologique que fondamental. Cependant, leurs tailles nanométriques, associées aux temps de vie sub-nanosecondes de leurs transitions optiques, rendent les mesures expérimentales très délicates.Ce travail de thèse propose une étude détaillée des mécanismes de déphasage et de couplage cohérent de complexes excitoniques fortement confinés dans des BQs InAs/GaAs individuelles. Pour réaliser ces mesures, j'ai développé une expérience de mélange à quatre ondes hétérodyne sensible à l'amplitude et à la phase du champ électrique émis par une BQ unique. Ce dispositif permet de mesurer le temps de vie et de cohérence d'un exciton unique, même en présence d'élargissement inhomogène. Pour augmenter l'interaction lumière-matière et l'efficacité d'extraction du signal, l'utilisation de nanostructures photoniques s'est avérée indispensable. La sensibilité optique du dispositif m'a permis d'étudier en détail les mécanismes d'interaction exciton-phonon, source importante de décohérence dans les solides, comme la formation du polaron acoustique, le couplage quadratique aux phonons acoustiques, et le déphasage induit pendant l'excitation. Par ailleurs, la réalisation de spectres bidimensionnels m'a permis de révéler le couplage cohérent entre différentes transitions excitoniques. Enfin, je présente un nouveau protocole de mélange multi-ondes permettant de contrôler la réponse cohérente d'un exciton unique que je propose d'appliquer sur une paire de BQs pour contrôler le couplage radiatif longue distance, étape fondamentale vers la réalisation d'une porte logique quantique dans les solides. / Decoherence in solids is a major issue towards the realization of a quantum processor based on semiconductor quantum dots (QDs) as optically active qubits. Measuring and controlling the optical coherence of such qubits is required in their fundamental studies, paving a way for technological applications. However, their nanometer size combined to the sub-nanosecond lifetime of their optical transitions, render experimental measurements very challenging.This thesis presents a detailed study of the dephasing mechanisms and the coherent coupling of excitonic complexes strongly confined in individual InAs/GaAs QDs. To achieve these measurements, I developed an heterodyne four-wave mixing experiment sensitive to the amplitude and phase of the electric field emitted by a single QD. With this setup one can measure the lifetime and the coherence time of a single exciton, even in the presence of inhomogeneous broadening. To increase the light-matter interaction and the extraction efficiency of the signal, the use of photonic nanostructures has proved to be necessary. The optical sensitivity of the setup allowed me to study in detail the mechanisms of exciton-phonon interaction, which is an important source of decoherence in solids, like the acoustic polaron formation, the quadratic coupling to acoustic phonons, and the excitation-induced dephasing. Furthermore, by inferring two-dimensional spectra, I demonstrate coherent couplings between various exciton complexes. Finally, I highlight a new multi-wave mixing protocol to control the coherent response of a single exciton, and I propose to employ it to control long-range radiative coupling between two QDs, which is a fundamental step towards achieving a quantum logic gate in solids.

Cette thèse est consacrée à de nouveaux phénomènes en physique liées au spin et à la topologie des quasi-particules lumière-matière dans des hétérostructures. Elle est divisée en quatre parties. Chapitre 1 donne un fond nécessaire et introduit les propriétés fondamentales des polaritons et des excitons indirects dans des puits quantiques couplés. Chapitre 2 est concentré sur la dynamique de spin et sur formation de défauts topologiques dans des systèmes aux excitons indirects. Les 2 derniers chapitres considèrent les structures basées sur les microcavités. Chapitre 3 est consacré à la dynamique de spin des polaritons dans des oscillateurs paramétriques optiques. Finalement, chapitre 4 étudie les réseaux des microcavités en forme des piliers et introduit l’isolant topologique polaritonique. / The present thesis manuscript is devoted to new phenomena in physics of light-matter quasiparticles in heterostructures, related to spin and topology. It is divided into four parts. Chapter 1 gives a necessary background, introducing basic properties of microcavity polaritons and indirect excitons in coupled quantum wells. Chapter 2 is focused on spin dynamics and topological defects formation in indirect exciton many-body systems. The last 2 chapters are related to microcavity-based structures. Chapter 3 is devoted to polariton spin dynamics in optical parametric oscillators. Finally, Chapter 4 studies pillar microcavity lattices and introduces the polariton topological insulator.

Ce travail de thèse porte sur la synthèse de cristaux liquides semiconducteurs, obtenus à partir de molécules associant des unités à caractère donneur-accepteur-donneur (DAD) et substituées aux deux extrémités par une chaîne oligosiloxane. Le fort pouvoir microségrégeant des oligosiloxanes a pour effet de stabiliser, pour l'ensemble des matériaux, une phase smectique unique (désordonnée) sur une gamme de température remarquablement large (>300°C). Pour des raisons de géométrie, les partie D et A doivent se nanostructurer en phase smectique pour conduire à la formation d'une structure à lamelles D/A alternées, favorable pour des applications photovoltaïques. Les matériaux ont fait l'objet de nombreuses études, notamment pour caractériser leurs propriétés structurales, photophysiques et de transport de charge. Ces matériaux ont ainsi révélé l'existence d'un transport de charge ambipolaire avec des valeurs de mobilité de l'ordre de 10-3 cm2/Vs en phase smectique. Les tests préliminaires de conversion photovoltaïque montre l'existence d'un très faible rendement, qui démontre l'importance d'un travail ultérieur d'optimisation des conditions de dépôts et du contrôle de l'orientation des couches smectiques sur les substrats.