<p dir="ltr">The increasing availability of spatio-temporal information in the form of detailed time-resolved images sampled at very high framing rates has resulted in a search for mathematical techniques capable of extracting and relaying the pertinent underlying physics governing complex flows. Analysis relying on the usage of a solitary spectral, correlation, or modal decomposition techniques to identify dynamically significant information from large datasets may give an incomplete description of these phenomena. Moreover, fully resolved spatio-temporal measurements of these complex flow fields are needed for a complete and accurate description across a wide spectrum of length and time scales. The primary goals of this dissertation are address these challenges in two key aspects: (1) to improve and demonstrate the novel application of complementary data analysis and modal decomposition techniques to quantify the dynamics of flow systems that exhibit intricate patterns and behaviors in both space and time, and (2) to make advancements in achieving and characterizing high-resolution and high-speed quantitative measurements of turbulent mixing fields.</p><p dir="ltr">In the first goal, two canonical flow fields are considered, including an acoustically excited co-axial jet and a bluff-body stabilized flame. The local susceptibility of a nonreacting, cryogenic, coaxial-jet, rocket injector to transverse acoustics is characterized by applying dynamical systems theory in conjunction with complementary wavelet-based spectral decomposition to high-speed backlit images of flow field. The local coupling of the jet with external acoustics is studied as a function of the relative momentum flux ratio between the outer and inner jets, giving a quantitative description of the dynamical response of each jet to external acoustics as a function of the downstream distance from the nozzle.</p><p dir="ltr">Bluff bodies are a common feature in the design of propulsion systems owing to their ability to act as flame holders. The reacting wake behind the bluff body consists of a recirculation bubble laden with hot-products and wrapped between separated shear layers. The wake region of a bluff body is systematically investigated utilizing a technique known as robust dynamic mode decomposition (DMD) to discern the onset of the thermoacoustic instability mode, which is highly detrimental to aerospace propulsion systems. The approach enables quantification of the spatial distribution and behavior of coherent structures observed from different flows as a function of the equivalence ratio.</p><p dir="ltr">As modal decomposition techniques employ a certain degree of averaging in time, a novel space-and-time local filtering technique utilizing the well-defined characteristics of wavelets is introduced with a goal of temporally resolving the spatial evolution of irregular flow instabilities associated with specific frequencies. This provides insight into the existence of transient sub-modal characteristics representing intermittencies within seemingly stable modes. The flow fields obtained from the same two canonical flows are interrogated to demonstrate the utility of the technique. It has been shown that temporally resolved flow features obtained from wavelet filtering satisfactorily track the same modal featured derived from DMD, but reveal sub-modal spatial distortions or local non-stationarity of specific modal frequencies on a frame-by-frame basis.</p><p dir="ltr">Finally, to improve the ability to study the dynamical behavior of complex flows across the full range of spatio-temporal scales present, advancements are reported in the spatial and temporal quantitative measurement of the scalar quantities in turbulent mixing fields utilizing 100 kHz planar laser-induced fluorescence (PLIF) and Rayleigh scattering imaging of acetone. The imaging system provided a resolution of 55 µm with a field-of-view mapping of 18.5 µm/pixel on the camera sensor, which is three times better spatial resolution than the previous reported work to-date for similar flow fields that were investigated at 1/10^th the current measurement rate. The power spectra of instantaneous mixture fraction fluctuations adhere to Kolmogorov's well-established -5/3 law, showing that the technique captures a significant range of dissipation scales. This observation underscores the ability to study mixing dynamics throughout the turbulent by fully resolving scalar fluctuations up to 30 kHz. This enhanced spatio-temporal resolution allows for a more detailed investigation of the dynamical behavior of turbulent flows with complex modal interactions down to the smallest diffusion limited mixing scales.</p>

<p dir="ltr">Two-dimensional (2D) perovskite semiconductors are an emerging family of hybrid materials featuring a built-in quantum well architecture which has gained much interest due to its potential as a promising candidate for next-generation photovoltaic and optoelectronic applications. To successfully integrate 2D perovskites as efficient devices, it is imperative that a thorough understanding of the fundamental properties these materials possess and how their complex heterostructures behave is established. However, to date, the synthetic challenges regarding high-quality crystals of these materials due to the structural complexity and the hybrid nature have impeded further progress in this area. Thus, we demonstrate a general method to construct tunable 2D organic semiconductor-incorporated perovskites (OSiP) by simultaneously manipulating slab thickness of the inorganic layers and conjugation length of the organic substituents. The energy band offsets and exciton dynamics at the organic-inorganic interfaces were elucidated using computational means and ultrafast spectroscopy, while lattice dynamics were quantified via temperature-dependent spectroscopy and X-ray diffraction studies. Results show that longer and more planar π-conjugated organic ligands induce a more rigid inorganic crystal lattice, which leads to suppressed exciton-phonon interactions and superior optoelectronic properties such as efficient lasing.</p><p dir="ltr">Furthermore, understanding ion migration in two-dimensional (2D) perovskite materials is key to enhancing device performance and stability as well. However, prior studies have been primarily limited to heat and light-induced ion migration. To investigate electrically induced ion migration in 2D perovskites, we construct a high-quality single crystal 2D perovskite heterostructure device platform with near defect-free van der Waals contact. While achieving real-time visualization of directional ion migration, we also uncover the unique behavior of halide anions inter-diffusing towards the opposite direction under prolonged bias. Confocal microscopy imaging reveals a halide migration channel that aligns with the crystal and heterojunction edges. After sustained ion migration, stable junction diodes exhibiting up to ~1000-fold forward to reverse current ratio are realized. Unraveling the fundamental properties of 2D OSiPs as well as ion migration in 2D perovskite heterostructures paves the way towards stable and efficient devices.</p>

<p>Laser-induced plasmas since their discovery in the 1960’s have found numerous applications in laboratories and industries. Their uses range from soft ionization source in mass spectroscopy, development of compact particle accelerator, and X-ray and deep UV radiation sources to diagnostic techniques such as laser-induced breakdown spectroscopy and laser electronic excitation tagging. In addition, the laser-induced plasma is important for studying of various nonlinear effects at beam propagation, such as laser pulse filamentation.</p> <p>This work deals with two challenging aspects associated with laser-induced plasmas. First is the study of Multi-Photon Ionization (MPI) as a fundamental first step in high-energy laser-matter interaction critical for understanding of the mechanism of plasma formation. The second is application of laser induced plasma for diagnostics of combustion systems.</p> <p>Numerous attempts to determine the basic physical constants of MPI process in direct experiments, namely photoionization rates and cross-sections of the MPI, were made; however, no reliable data was available until now, and the spread in the literature values often reached 2–3 orders of magnitude. This work presents the use of microwave scattering in quasi-Rayleigh regime off the electrons in the laser-induced plasma as method to measure the total number of electrons created due to the photoionization process and subsequently determine the cross-sections and rates of MPI. Experiments were done in air,<i> O₂, Xe, Ar, N₂, Kr</i>, and <i>CO</i> at room temperature and atmospheric pressure and femtosecond-laser pulse at 800 nm wavelength was utilized. Rayleigh microwave scattering (RMS) technique was used to obtain temporally resolved measurements of the electron numbers created by the laser. Numbers of electrons in the range 3 × 10⁸–3 × 10¹² were produced by the laser pulse energies 100–700 <i>μ</i>J and corresponding electron number densities down to about 10¹⁴ cm^-3 in the center of laser-induced spark were observed. After the laser pulse, plasma decayed on the time scale from 1 to 40 ns depending on the gas type and governed by two competing processes, namely, the creation of new electrons from ionization of the metastable atoms and loss of the electrons due to dissociative recombination and attachment to oxygen. </p> <p>Diagnostics of combustion at high pressures are challenging due to increased collisional quenching and associated loss of acquired signal. In this work, resonance enhanced multiphoton photon ionization (REMPI) in conjunction with measurement of generated electrons by RMS technique were used to develop diagnostics method for measuring concentration of a component in gaseous mixture at elected pressure. Specifically, the REMPI-RMS diagnostics was developed and tested in the measurements of number density of carbon monoxide (<i>CO</i>) in mixtures with nitrogen (<i>N₂</i>) at pressures up to 5 bars. Number of REMPI-induced electrons scaled linearly with <i>CO</i> number density up to about 5×10¹⁸ cm^-3 independently of buffer gas pressure up to 5 bar, and this linear scaling region can be readily used for diagnostics purposes. Higher <i>CO</i> number densities were associated laser beam energy loss while travelling through the gaseous mixture. Four (4) energy level model of <i>CO</i> molecule was developed and direct measurements of the laser pulse energy absorbed in the two-photon process during the passage through the <i>CO</i>/<i>N₂</i> mixture were conducted in order to analyze the observed trends of number of REMPI-generated electrons with <i>CO</i> number density and laser energy.</p>

<p>Constructive elastic microwave scattering, or, historically, coherent microwave scattering (CMS), refers to the inference of small plasma object characteristics via in-phase electromagnetic scattering – and has become a valuable technique in applications ranging from photoionization and electron-loss rate measurements to trace species detection, gaseous mixture and reaction characterization, molecular spectroscopy, and standoff measurement of local vector magnetic fields in gases through magnetically-induced depolarization. Notable advantages of the technique include a high sensitivity, good temporal resolution, low shot noise, non-intrusive probing, species-selectivity when coupled with resonance-enhanced multiphoton ionization (REMPI), single-shot acquisition, and the capability of time gating due to continuous scanning.</p> <p>Originally, the diagnostic was used for the measurement of electron total populations and number densities in collisional, weakly-ionized, and unmagnetized small plasma objects – so called collisional scattering. However, despite increased interest in recent years, the technique’s applicability to collisionless plasmas has remained relatively unexplored. This dissertation intends to expand upon the theoretical, mathematical, and experimental basis for CMS and demonstrate the constructive Thomson & Rayleigh scattering regimes for the first time. Furthermore, this work seeks to explore other novel and relevant capabilities of CMS including electron momentum-transfer collision frequency measurements via scattered phase information and spatially-resolved electron number characterizations of elongated plasma filament structures.</p> <p>This dissertation additionally leverages the technique to diagnose microplasmas and situations of particular interest. Primarily, photoionization (PI) – including UV resonance-enhanced multiphoton ionization, non-resonant visible PI, and mid-IR tunneling ionization in gaseous media. Such processes bear importance to studies on nonequilibrium plasmas, soft ionization in mass spectrometry, the development of compact particle accelerators, X-ray and deep UV radiation sources, laser-assisted combustion, laser-induced breakdown spectroscopy, species detection, mixture characterization and spectroscopy, studies on nonlinear beam propagation (filamentation, self-trapping and pulse splitting, dispersion, modulation instabilities), and so on. Finally, the application of CMS to ion thrusters is demonstrated.</p>

Dans cette thèse, nous avons appliqué les outils modernes de la théorie des systèmes dynamiques à l'étude des lasers. Le but de ce travail était de mieux comprendre les sources cohérentes existantes en vue de les améliorer et de proposer de nouveaux mécanismes d'amplification lumineuse.<p><p>Motivé par de récentes expériences menées sur des lasers miniatures avec absorbant saturable, nous en avons repris la description théorique. Les nouvelles valeurs de paramètres suggérées par l'expérience nous ont amenés à découvrir de nouveaux comportements dynamiques pour ces systèmes. En particulier, nous avons décrit comment l'intensité délivrée par ces lasers devenait temporellement sinusoïdale, puis impulsionnelle sur un très petit intervalle de paramètres.<p><p>Par la connaissance acquise du laser à absorbant saturable, nous avons pu comprendre comment s'établissait un régime impulsionnel semblable dans un autre laser. Il s'agissait du laser multimode à pompage longitudinalement inhomogène. Il est apparu en effet qu'une partie du milieu emprisonné dans la cavité optique agissait à la manière d'un absorbant saturable, déstabilisant ainsi l'émission continue de ce laser. Nous avons également montré que, dans certaines circonstances, son état dynamique présentait des effets de mémoire. Une autre propriété importante de la dynamique du laser multimode a été mise en évidence: pour de petites perturbations, l'intensité totale présente un comportement plus régulier que les intensités modales prises séparément.<p><p>Ce type intrigant d'auto organisation fut rencontré plus tard, lorsque nous avons envisagé la dynamique d'un réseau de lasers à semi conducteur couplés par un feedback optique. Le retard accumulé par la lumière au cours de ce feedback est un paramètre essentiel du problème. Ce système important sur le plan technologique s'est révélé extrêmement riche sur le plan dynamique. Nous avons pu montrer que plus le retard était grand, plus les lasers avaient tendance à se synchroniser. Cela fut observé aussi bien en régime continu qu'en régime périodique ou chaotique. Par une telle synchronisation, la qualité du rayon optique émis par le réseau de lasers augmente spectaculairement, élargissant par là ses possibilités d'application.<p><p>Au début des années 1990, les physiciens commencèrent à étudier systématiquement les effets d'interférence quantique dans l'interaction lumière matière. Ceci faisait suite à l'annonce fracassante que de tels effets devaient permettre de construire des lasers sans inversion de population. Récemment, une série d'expériences a montré que de telles interférences quantiques étaient à l’œuvre dans le laser miniature LNP. Une partie de cette thèse y fut consacrée. Nous avons montré que le comportement dynamique observé résultait d'un renforcement quantique de l'absorption stimulée par les niveaux énergétiques inférieurs.<p><p>Nous avons poursuivi notre étude des effets d'interférence quantique sur un schéma électronucléaire. Nous avons montré que pour ce système, un rayon gamma peut être amplifié sans inversion de population. Ce résultat est très important, compte tenu du fait qu'une telle inversion est techniquement impossible à réaliser pour ces très hautes fréquences électromagnétiques, empêchant jusqu'ici la réalisation de lasers gamma. Afin d'atteindre l'amplification sans inversion, un rayonnement d'appoint dans le domaine optique s'avère nécessaire. Tenant compte de la décroissance de ce champ optique en cours de propagation, et donc de la diminution des effets quantiques associés, nous avons déterminé une distance optimale de propagation. Au-delà de cette distance, l'amplification se mue en absorption. Une telle information est dès lors cruciale sur le plan expérimental.<p> / Doctorat en sciences appliquées / info:eu-repo/semantics/nonPublished

<div>The interactions of femtosecond lasers with gold targets were investigated with a numerical method combining molecular dynamics (MD) and the two-temperature model (TTM). Previous works using MD-TTM method did not consider all the thermodynamic parameters and the interatomic potential dependent of the electron temperature simultaneously. Therefore, we developed a LAMMPS function to achieve this. To accurately capture the physics behind the interactions, we also included the electron blast force from free electron pressure and the modified Fourier law with steep electron temperature gradient in our model. For bulk materials, a stress non-reflecting and heat conducting boundary is added between the atomistic and the continuum parts. The modified boundary force in our study greatly reduces the reflectivity of the atomistic-continuum boundary compared with its original form. Our model is the first to consider all these factors simultaneously and manage to predict four femtosecond laser ablation phenomena observed in the experiments. </div><div><br></div><div>In this dissertation, the thermodynamic parameters in the two-temperature model were extensively explored. We considered three different approaches to calculate these parameters: namely interpolation, <i>ab initio</i> calculation, and analytical expression. We found that simple interpolation between solid state and plasma state could lead to high level of inaccuracy, especially for electron thermal conductivity. Therefore, <i>ab initio</i> calculation and analytical expression were used for the calculation of the thermodynamic parameters in more advanced studies. The effects of electron thermal conductivity and electron-phonon coupling factor on electron and lattice temperatures were analyzed.</div><div><br></div><div>Our studies considered electron temperature dependent (ETD) and electron temperature independent (ETI) interatomic potentials. The ETI interatomic potential is easier to implement and therefore it is used in our phase change study to investigate the effects of target thickness on melting. Homogeneous melting occurred for thin films, while melting can be observed through the movement of the solid-liquid interface in thick or bulk materials. However, the ETI potential overestimated the bond strength at high temperatures. Therefore, ablation process was studied with the ETD potential. Three ablation mechanisms were found in our simulations at different laser fluences. Short nonthermal ablation was only observed at the ablation threshold. With increasing laser fluence, spallation was then seen. In high laser fluence regime, phase explosion occurred on the surface and coexisted with spallation.</div><div><br></div><div>Lastly, we researched on the effects of the delay time between two femtosecond laser pulses. Various delay times did not have much influence on melting depth. In low laser fluence regime, with increasing delay time, the target went through nonthermal ablation, to spallation and to no ablation. In high laser fluence regime, longer delay time encouraged phase explosion while suppressed spallation.</div>