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.

Nesta tese, estudamos o processo de absorção multifotônica em polímeros e resinas poliméricas, abordando tanto aspectos fundamentais quanto aplicados. Com relação aos aspectos fundamentais, estudamos processos de absorção multifotônica (absorção de dois, três e quatro fótons) no polímero conjugado MEH-PPV (poly(2-methoxy-5-(2´-ethylhexyloxy)-1,4- phenylenevinylene)), utilizando a técnica de Varredura-Z com pulsos ultracurtos. Através desta técnica, determinamos o espectro da absorção de dois, três e quatro fótons do MEHPPV. As seções de choque de absorção de multi-fótons correspondentes a cada processo foram determinadas através do ajuste das curvas experimentais com um conjunto de equações desenvolvidas neste trabalho. Os resultados obtidos permitiram traçar relações entre os espectros não lineares e os níveis de energia do polímero. Na vertente mais aplicada do projeto, estudamos a fotopolimerização de resinas acrílicas através do processo de absorção de dois fótons. Devido ao confinamento espacial da polimerização, graças à absorção de dois fótons, este método permite a confecção de micro-estruturas complexas para diversas aplicações tecnológicas. Além da fabricação de microestruturas convencionais não dopadas, neste trabalho desenvolvemos uma metodologia que possibilita a fabricação de microestruturas dopadas com MEH-PPV, visando a produção de micro-elementos fluorescentes para dispositivos fotônicos, e microestruturas dopadas com quitosana, um polímero biocompatível que pode ser utilizado em aplicações médicas e biológicas. / In this thesis we have studied the multi-photon absorption process in polymers and polymeric resins, exploiting its fundamental as well as technological aspects. Regarding the fundamental aspects, we have studied the multi-photon absorption (two-, three- and four-photon absorption) in the conjugated polymer MEH-PPV (poly(2-methoxy-5-(2´-ethylhexyloxy)-1,4-phenylenevinylene)), by using the Z-scan technique with ultrashort laser pulses. Through this technique, we determined the two-, three- and four-photon absorption spectra of MEH-PPV. The multi-photon absorption cross-sections, corresponding to each specific process, have been determined by fitting the experimental data with a set of equations developed in this work. The results allowed us to correlate the nonlinear absorption spectra to the energy level of the polymer. On the technological side of this thesis, we have investigated the photopolymerization of acrylic resins by two-photon absorption. Because of the spatial confinement of the polymerization, resulting from the two-photon excitation, this method allows the fabrication of complex microstructures which can be used for several technological applications. In addition to the fabrication of undoped microstructures, in this work we have developed a methodology that allows the fabrication of microstructures doped with MEHPPV, aiming the production of fluorescent micro-elements for photonics applications, and microstructures doped with chitosan, a biocompatible polymer, that can be used for medical and biological applications.

<p>Ultrafast laser-based diagnostic techniques are powerful tools for the detailed understanding of highly dynamic combustion chemistry and physics. The ultrashort pulses provide unprecedented temporal resolution along with high peak power for broad spectral range−ideal for nonlinear signal generation at high repetition rate−with applications including next-generation combustors for gas turbines, plasma-assisted combustion, hypersonic flows and rotating detonation engines. The current work focuses on advancing (i) femtosecond (fs) two-photon laser-induced fluorescence, and (ii) hybrid femtosecond/picosecond vibrational and rotational coherent anti-Stokes Raman scattering (fs/ps RCARS and VCARS) to higher pressures for the first time. </p><p>Quantitative single-laser-shot kHz-rate concentration measurements of key atomic (O-atom) and molecular (CO) species is presented using femtosecond two-photon laser-induced fluorescence (TP-LIF) for a range of equivalence ratios and pressures in diffusion flames. A multitude of signal-interfering sources and loss mechanisms−relevant to high-pressure fs TP-LIF applications−are also quantified up to 20 atm to ensure high accuracy. The pressure scaling of interferences take into account degradation, attenuation and wave-front distortion of the excitation laser pulse; collisional quenching and pressure dependent transition line-broadening and shifting; photolytic interferences; multi-photon ionization; stimulated emission; and radiation trapping. </p><p>Hybrid fs/ps VCARS of N₂ is reported for interference-free temperature measurement at 1300-2300 K in high-pressure, laminar diffusion flames up to 10 atm. A time asymmetric probe pulse allowed for detection of spectrally resolved CARS signals at probe delays as early as ~200-300 fs while being independent of collisions for the full range of pressures and temperatures. Limits of collisional independence, accuracy and precision of the measurement is explored at various probe-pulse delays, pressures and temperatures. </p><p> </p><p>Additionally, a novel all diode-pumped Nd:YAG amplifier design is presented for generation of time-synchronized ps-probe pulses for hybrid fs/ps RCARS of N₂. High-energy, nearly transform-limited, single-mode, chirp-free ps probe-pulses are generated at variable pulsewidths. The detailed architecture and characterization of the laser is presented. kHz-rate RCARS thermometry is presented up to 2400 K. Excellent spatial, spectral, and temporal beam quality allowed for fitting the theoretical spectra with a simple Gaussian model for the probe pulse with temperature accuracies of 1-2%. </p> <p><br></p>