For many years, microbubbles have been used as ultrasound contrast agents to improve the quality of diagnostics, seeing that they produce more backscattering ultrasound than blood does. Novel types of microbubbles and increased knowledge about their different behaviors have led to other suggested areas of use. One notable example is the poly-vinyl alcohol (PVA) microbubble, which has been discovered to have a unique fracturing mechanism referred to as the pumping-out behavior. The PVA microbubble has the potential to be used, for instance, in local drug delivery of therapeutic gases, but further studies are needed. In this study, the aim was to develop a tool for imaging the pumping-out behavior of the PVA microbubbles. A linear transducer connected to the programmable Verasonics Research System operated by MatLab software was used to achieve it. The designed ultrasound sequences were tested on a tissue-mimicking phantom containing one vessel filled with PVA microbubbles and one with degassed water. The design was divided into two steps. First, an ultrafast imaging sequence, based on plane waves, was developed to achieve adequate acquisition rate for detecting escaping air from the microbubbles. Furthermore, coherent compounding was implemented to compensate for some of the loss in image quality due to the use of plane waves instead of focused waves. The second step of the design was to combine the imaging sequence with destruction pulses so that the pumping-out behavior could be imaged. The designed ultrasound sequence was evaluated by calculating the mean pixel intensities, contrast-to-tissue ratio (CTR), and contrast-to-noise ratio (CNR) of different regions of interest (ROI) in the acquired images. The results of this project agree with the result previously reported in a study of PVA microbubbles made by Kothapalli et al.. Thus, the developed tool can image the pumping-out behavior. However, further improvements to the imaging tool, such as use of a contrast specific method, is recommended for it to become more reliable and useful. In conclusion, the developed imaging tool works for imaging the pumping-out behavior, but improvements should be made. With a useful imaging tool, further studies can be performed to understand the parameters affecting the pumping-out behavior. In the end, the PVA microbubbles can possibly be used as, for example, local drug deliverers in the clinic.

<p>Mechanical oscillating drills and saws are used in orthopaedic surgery to cut bone and develop screw-holes; however, their use causes friction resulting in significant thermal damage. Ultrashort pulsed lasers appear well-suited to replace traditional tools as they have the ability to efficiently remove bone tissue while causing only minimal collateral damage. Laser ablation also has the added advantages of: (i) no mechanical vibration; (ii) minimal invasiveness; and (iii) small focus spot size. In this thesis work, we experimentally investigated a few key aspects of ultrashort laser ablation of bone tissue.</p> <p>The ablation threshold of unaltered bone was measured using the <em>D</em>²technique and found to range from 1.66 J/cm²± 0.87 J/cm² to 2.37 J/cm²± 0.78 J/cm² depending on incident pulse number. The reduction in ablation threshold with pulse number was an indication of an incubation effect. Using a power law model, the incubation coefficient, ζ, was measured to be 0.89 ± 0.03.</p> <p>The effect of specific laser parameters and drilling protocols on ablation efficiency was also characterized. For ultrashort pulses (≤10 ps), the removal rate was found to be inversely related to the pulse duration; however, irradiation with 5-10 ps pulses were also shown to result in significant tissue removal. With a pulse repetition rate of 1 kHz, the removal rate was observed to be highest when ablating with 50-100 pulses per spot.</p> <p>Larger volumes (>1 mm³) of bone tissue were removed using laser scanning procedures. A series of scanned concentric circles produced a structure ~2.4 mm deep; however, ablated side-lobes were present at oblique angles to the incident beam. A two-layer structure subsequently produced no side-lobes. The ablative precision in trabecular bone was observed to be less than cortical bone. Using mimicked Nd:YAG laser parameters, cylindrical drilling produced craters significantly less deep than those achieved with a typical Ti:Sapphire configuration. The ability to drill large-scale holes using low average pulse energies and optimized scanning procedures will alleviate the stringent requirements for optical components in clinical practice.</p> / Master of Science (MSc)

MXenes, a new class of two-dimensional (2D) materials, have recently demonstrated impressive optoelectronic properties associated with its ultrathin layered structure. Particularly, Ti3C2Tx, the most studied MXene by far, was shown to exhibit intense surface plasmons (SPs), i.e. collective oscillations of free charge carriers, when excited by electromagnetic waves. However, due to the lack of information about the spatial and energy variation of those SPs over individual MXene flakes, the potential use of MXenes in photonics and plasmonics is still marginally explored. Hence, the main objective of this dissertation is to shed the light upon the plasmonic behavior of MXenes at the nanoscale and extend their use beyond their typical electrochemical applications. To fulfill our objective, we first elucidated the underlying characteristics governing the plasmonic behavior of MXenes. Then, we revealed the existence of various tunable SP modes supported by different MXenes, i.e. Ti3C2Tx and Mo2CTx, and investigated their energy and spatial distribution over individual flakes. Further, we fabricated an array of MXene-based flexible photodetectors that only operate at the resonant frequency of the SPs supported by MXenes. We also unveiled the existence of tunable SPs supported by another 2D nanomaterial (i.e. MoO2) and juxtaposed its plasmonic behavior with that of MXenes, to underline the uniqueness of the latter. Noteworthy, as in the case of MXenes, this was the first progress made on studying specific SP modes supported by MoO2 nanostructures. In this part of the dissertation, we were able to identify and tailor multipolar SPs supported by MoO2 and illustrate their dependence on their bulk band structure. In the end, we show that, on the contrary, SPs in MXenes are mainly controlled by the surface band structure. To confirm this, we selectively altered the subsurface band structure of Ti3C2Tx and modulated its work function (from 4.37 to 4.81 eV) via charge transfer doping. Interestingly, thanks to the unchanged surface stoichiometry of Ti3C2Tx, the plasmonic behavior of Ti3C2Tx was not affected by its largely tuned electronic structure. Notably, the ability to attain MXenes with tunable work functions, yet without disrupting their plasmonic behavior, is appealing to many application fields.

<p dir="ltr">Some of the simplest molecules that are found in abundance in nature, like oxygen, nitrogen, carbon dioxide and water can be playgrounds for complex quantum mechanical phenomenon. Although we can calculate their static properties, like binding energies, equilibrium geometries and ionization/decay rates with extraordinary precision, their dynamics offer new avenues for exploration. Although analytical techniques have been successfully applied in studying single-particle and many-particle systems, few-particle systems like simple molecules are still best understood through a combination of numerical calculations and experimental work. However, the small size of these molecules endows them with dynamics that occur on timescales of a few picoseconds to a few attoseconds, making their experimental study challenging. The overarching goal of this work is the study of such ‘ultrafast’ dynamics in excited state molecules/atoms, by developing and demonstrating novel optical probes of quantum dynamics.</p><p dir="ltr">One way to probe ultrafast dynamics in molecules is by measuring their nonlinear optical response. Such a measurement can potentially track the evolution of the symmetries of excited molecules, shedding light on their transient dynamics. We start chapter 1 with a brief discussion of the formalism behind nonlinear optical spectroscopy. Direct measurement of ultrafast (and ultraweak) optical pulses is discussed as a useful probe of nonlinear processes. After presenting preliminary results on direct electric field reconstruction, experimental work on measuring emitted nonlinear electric fields from impulsively aligned molecules is discussed. In such an experiment, however, contributions from both aligned and unaligned molecules are present, and new experimental capabilities had to be developed to disentangle and measure the ultraweak signal from aligned molecules. Following a detailed discussion of the developed measurement capabilities, results from experiments done on aligned carbon dioxide and nitrogen molecules are discussed.</p><p dir="ltr">Unlike solids, where electronic states can be excited with visible/UV light, binding energies in isolated atoms/molecules are on the order of electron-volts (eVs), and they need vacuum-ultraviolet (VUV) extreme-ultraviolet (EUV) light to excite electronically. Polyatomic molecules, like ethylene, when excited to an electronic state with VUV light, often relax back to the ground state by redistributing energy to their internal degrees of freedom non-adiabatically. These relaxation pathways are important in many chemical and biological systems, and control the yield of chemical reactions ranging from elementary reactions involving few atoms to large biomolecules such as DNA and proteins. For instance, in the photochemical reaction of the protein Rhodopsin, considered to be the primary event in human vision. In chapter 2 we discuss progress made towards extending nonlinear response measurements to study ultrafast dynamics in electronically excited molecules, using a high-harmonic VUV source. Details about the design of the high-harmonic generation beamline, and preliminary experimental data are presented. In chapter 3 we discuss preliminary theoretical work on the development of an EUV entangled-photon source, using two-photon emission from the metastable 2s state in neutral Helium. Such a source, if demonstrated, can possibly even extended to the zeptosecond regime in the future.</p>

Thulium (Tm)-doped ultrafast fiber lasers with emission wavelengths around 2 μm are desirable sources for scientific, industrial, medical, and environmental applications and flexible testbeds for investigating nonlinear pulse dynamics. Although exceptional research attention has been drawn by Tm-doped ultrafast fiber lasers in recent years, their designs and dynamics are significantly less explored compared to other fiber laser systems. Despite the broad emission spectrum of Tm-doped fibers, power scaling of Tm-doped ultrafast fiber lasers has been limited at shorter wavelengths of their emission spectrum (<1920 nm) due to challenges including signal re-absorption. However, compact, high-energy ultrafast sources at these less-exploited wavelengths can enable various applications including nonlinear microscopy. Further, due to the challenges of implementing real-time characterization around 2 μm, transient nonlinear pulse dynamics have rarely been reported from Tm-doped ultrafast fiber lasers. Resolving these dynamics can not only provide insights into new laser designs but also guide the generation of novel pulse profiles which can benefit a wide range of applications depending on their parameters. This dissertation focuses on developing various novel Tm-doped ultrafast fiber laser systems with unprecedented performance: High-energy operation is demonstrated at less-exploited wavelengths and unique waveforms are generated with their nonlinear dynamics investigated in real-time. First, a high-energy (394-nJ) Tm-doped chirped-pulse-amplification fiber laser system is designed and optimized for operation at the wavelength of 1900 nm and supports the generation of 950-nm ultrashort (390-fs) pulses via frequency-doubling. The system represents the highest pulse-energy (138 nJ) in the femtosecond regime for any fiber-based systems around this wavelength to date, which can be highly attractive for two-photon microscopy with spatiotemporal-multiplexing. To gain deeper insights into the operation of ultrafast Tm-doped fiber lasers, various new nonlinear dynamics are investigated by a home-built real-time characterization setup based on dispersive Fourier transform for 2 μm pulses: A new mode-locking regime is demonstrated which can deliver both up-chirped and close-to-chirp-free dissipative pulses with a 10-fold difference in their pulse energies/durations, providing a versatile source that can switch between different pulse profiles. Following that, soliton molecules with unique partial spectral modulation patterns are synthesized based on two dissimilar pulses from the same cavity, which represent an interesting analogy to ‘heteronuclear’ chemical molecules and hold great potential for optical information processing. Further, mode-locking evolution between dissimilar coherent pulses are studied in Tm-doped ultrafast fiber lasers. Finally, combining both high-energy operation and novel waveform-generation, we present a Tm-doped fiber laser source delivering amplified (~ 200 nJ) noise-like pulses without requiring any feedback mechanism. / 2025-09-10T00:00:00Z

<p>This dissertation discusses theoretical methods for describing photoionization in different systems in the context of time-dependent and time-independent non-relativistic and time-independent relativistic systems. We introduce a multichannel quantum defect theory (MQDT) model for describing photoionization in the context of pump-probe experiments. The basics of MQDT are introduced and specialized to the argon atom. Two energy regimes are studied in detail and compared to the experiment: (i) a perturbative calculation describing the dynamics of an autoionizing wave packet, (ii) a time-resolved calculation describing the two-photon ionization of a deeply bound wave packet. In both cases, the model accurately describes the relative ionization with respect to the two spin-orbit split thresholds of the ion and the oscillations shown in the delay between the pump and probe. We finalize with a brief presentation, which is primarily pedagogical, of how to use MQDT inside a finite box.</p> <p>Next, we use MQDT to describe the ytterbium atom in different energy regimes and varying degrees of approximation. The motivation behind this lies in the context of quantum information science, but our study is only concerned with calculating atomic properties. We start with a minimal MQDT model to describe the data observed in the experiment, followed by the presentation of an ab initio two-electron model. Both models compare very well to the experiment, and the ab initio method compares favorably with older spectroscopic results. In addition, we show unpublished results that incorporate the hyper-fine effects into the approximate model.</p> <p>Finally, we present an implementation of the two-electron variational R-matrix method for the Dirac equation, including the complete derivation of the solution of the Dirac equation in a central potential. We provide explicit analytic forms for the solutions of the Coulomb potential and use them to derive the generalized quantum defect parameters. A discussion of the variational R-matrix method for the Dirac equation in single and multichannel contexts is presented, with sample calculations for the beryllium and radium atoms. A chapter that summarizes and points to future work for each one of the projects concludes the work.</p>

Semiconductor lasers are considered essential for the advancement in the field of photonics where compact and energy-efficient lasers are necessary. Advancements in integrated photonic technologies will help push the performance of semiconductor lasers in the coming years and expand the technology to several other applications. Semiconductor lasers offer several key features such as high energy efficiency, mass production, availability at a myriad of wavelengths, and high integration capabilities. However, limitations in noise performance, pulse energy, and duration hold back semiconductor lasers from being utilized to their full potential. This dissertation reviews the utilization and development of external techniques that enable semiconductor mode-locked lasers to be used in multi-photon imaging and microwave photonic applications. We first review a two-color external cavity mode-locked laser system operating at wavelengths 834 nm and 974 nm that can generate synchronized picosecond pulses with peak powers exceeding 80 W and 100 W respectively. We verify the feasibility of this system to induce non-linear processes by demonstrating two-photon excitation in commercially available dyes. Next, we introduce the concepts of optical injection locking and discuss the development of a multi-tone optical self-injection locking technique to improve the noise performance and optical linewidth of a chip-scale InP based mode-locked laser. We utilize a Fabry-Perot etalon as the optical comb filter, which also serves to suppress the super-mode noise that arises from external cavity feedback. In addition to this, we also implement a coupled opto-electronic loop and reference it to an external RF source demonstrating exceptional timing stability. This approach along with the usage of fully integrated and ultra-compact components in subsequent versions has the potential to realize compact frequency comb lasers for microwave photonic and other practical applications.

<p dir="ltr">This thesis advances the methodologies of quantum state tomography (QST) to validate and optimize quantum processing on Noisy Intermediate-Scale Quantum (NISQ) devices, crucial for the transition to practical quantum systems. Inspired by recent advancements in the field, we propose a novel QST method based on the maximal entropy formalism, specifically addressing scenarios with incomplete measurement sets to provide a robust framework for state reconstruction. We extend this formalism to an informationally complete (IC) set of observables and introduce a variational approach for quantum state preparation, easily implementable on near-term quantum devices. Our developed maximal entropy-based QST protocol is applied to ultrafast molecular dynamics specifically for studying photoexcited ammonia molecule, enabling direct measurement and manipulation of electronic quantum coherences and exploring entanglement effects in molecular systems. Through this approach, we achieve a groundbreaking milestone by, for the first time, constructing the entanglement entropy of the electronic subsystem - an otherwise inaccessible metric. In doing so it also provides the first physical interpretation of the maximal entropy parameters in an experimental setting and highlights the potential for feedback between time-resolved quantum dynamics and quantum information science. Furthermore, building upon our advancements in state tomography, we propose a variational quantum algorithm for Hamiltonian learning that leverages the time dynamics of observables. Additionally, we reverse engineer the maximal entropy approach and demonstrate the use of entropy to refine the traditional geometric Brownian motion (GBM) method for better capturing real system complexities by addressing its log-normality restrictions, which opens new avenues for quantum sampling techniques. Through these contributions, this thesis showcases the Maximal Entropy formalism’s efficacy in QST and set the stage for future innovations and applications in cutting-edge quantum research.</p>

<p dir="ltr">Ultrafast optics is an important field of study for chemistry and physics, providing new information on the dynamics of matter and electrons. In this thesis I describe my work on ultrafast laser systems. The two main systems discussed are a high harmonic generated extreme ultraviolet system and a terahertz spectroscopy system. The first half describes the importance and background of both as well as how these systems are set up. The second half describes my work in designing and implanting these systems, and my work in constructing components for the operation of both.</p>

La technique d’optique ultra-rapide pompe-sonde, qui repose sur l’emploi de lasers à impulsion ultracourte(femtoseconde), permet de déclencher et étudier des processus ultrarapides dans la matière. L’acoustique picoseconde concerne pour sa part l’étude des processus de génération et détection de phonons acoustiques haute fréquence ainsi quel’analyse des nanomatériaux avec ces phonons (nanoéchographie). Les travaux de recherche de cette thèse avaient pourbut l’étude des couplages électronphonon acoustique dans le matériau ferroélectrique BiFeO3 par acoustique ultrarapide. Nous avons pu mettre en évidence que selon l’orientation du cristal photoexcité, l’émission des phonons acoustiques cohérents longitudinaux (LA) et transverses (TA) pouvait être modulée. De manière spectaculaire, nous avons purévéler un couplage électron-phonon acoustique transverse très efficace comme cela n’avait jamais été observé jusqu’alors dans les métaux, semiconducteurs ou nanostructures artificielles. Une étude détaillée indique que le mécanismepiézoélectrique inverse semble être le moteur de ce couplage électron-phonon (Lejman et al, Nature Communications, 2014). Dans une seconde partie, nous avons montré que BFO, ainsi qu’un autre ferroélectrique biréfringent LiNbO3 (LNO), peuvent être utilisés pour la conversion de mode ultra-rapide par processus acousto-optique (manipulation de la polarisation de la lumière à l’échelle de la picoseconde avec des phonons acoustiques). Cet effet, jamais mis enévidence jusqu’alors dans le domaine GHz, pourrait potentiellement être exploité dans de nouveaux dispositifs photoniques/phononiques pour des modulations acousto-optiques à haute cadence. / Ultrafast optical pump-probe technique, by exploiting ultrashort laser pulses (femtosecond), allows to initiate and monitor ultrafast processes in matter. Picosecond acoustics is a research field that focuses on the generation and detection mechanisms of high frequency coherent acoustic phonons in different media, as well as on their application in testing of nanomaterials and nanostructures. This PhDs research project was devoted to study of electron-acoustic phonon coupling in ferroelectric BiFeO3 (bismuth ferrite, BFO) by ultrafast acoustics. We have evidenced that depending on the BFO crystal orientation it was possible to tune the coherent phonons spectrum with in particular variable amplitude of longitudinal (LA) and transverse (TA) acoustic modes. In some grains with particular crystallographic orientations much stronger TA than LA signal was observed. Spectacularly, we have revealed an efficient coupling between electron and transverse acousticphonon. Such high ratio never reported before in any metal, semiconductor or nanostructure before, can be principally attributed to the photoinduced inverse piezoelectric effect (Lejman et al Nature Communications 2014). In a second part, we have shown that BFO as well as another birefringent ferroelectric LiNbO3 (LNO) can be used for ultrafast acousto-optic modeconversion (manipulation of light polarization at the picosecond time scale with coherent acoustic phonons). This effect, never reported at GHz up to now, can be potentially applied in photonics for ultrafast manipulation of light polarization bycoherent acoustic phonons in next generation photonic/phononic devices.