In this study¡Awe apply the broad bandwidth and high energy pulse of ultrafast laser to experiment on RF OBIC and second harmonic generation. In this paper a novel method is presented for characterizing high frequency response and behavior of ultra high-speed photosensitive semiconductor devices and the set-up is capable of generating excitation at RF bandwidths of greater than 1.8 THz. In addition¡Athe collagen of dentine is able to generate the second harmonic in the ultraviolet region, so we develop a high performance transmission mode laser scanning microscope for obtaining SHG images of a tooth slice. We also study wavelength dependence and polarization dependence.

The invention of chirped-pulse amplification (CPA) in 1985 led to a tremendous increase in obtainable laser pulse peak intensities. Since then, several table-top, Ti:sapphire-based CPA systems exceeding the 100 TW-level with more than 10 W average power have been developed and several systems are now commercially available. Over the last decade, the complementary technology of optical parametric chirped-pulse amplification (OPCPA) has improved in its performance to a competitive level. OPCPA allows direct amplification of an almost-octave spanning bandwidth supporting few-cycle pulse durations at center wavelengths ranging from the visible to the mid-IR. The current record in peak power from a table-top OPCPA is 16 TW and the current record average power is 22 W. High energy, few-cycle pulses with stabilized carrierenvelope phase (CEP) are desired for applications such as high-harmonic generation (HHG) enabling attoscience and the generation keV-photon bursts. This dissertation conceptually, numerically and experimentally describes essential aspects of few-cycle OPCPA, and the associated pump beam generation. The main part of the conducted research was directed towards the few-cycle OPCPA facility developed in the Laser Plasma Laboratory at CREOL (University of Central Florida, USA) termed HERACLES. This facility was designed to generate few-cycle pulses in the visible with mJ-level pulse energy, W-level average power and more than 100 GW peak power. Major parts of the implementation of the HERACLES facility are presented. The pump generation beam of the HERACLES system has been improved in terms of pulse energy, average power and stability over the last years. It is based on diode-pumped, solid-state amplifiers with picosecond duration and experimental investigations are presented in detail. A iii robust system has been implemented producing mJ-level pulse energies with ~100 ps pulse duration at kHz repetition rates. Scaling of this system to high power (>30 W) and high peak power (50-MW-level) as well as ultra-high pulse energy (>160 mJ) is presented. The latter investigation resulted in the design of an ultra-high energy system for OPCPA pumping. Following this, a new OPCPA facility was designed termed PhaSTHEUS, which is anticipated to reach ultra-high intensities. Another research effort was conducted at CELIA (Univeristé de Bordeaux 1, France) and aimed towards a previously unexplored operational regime of OPCPA with ultra-high repetition rates (10 MHz) and high average power. A supercontinuum seed beam generation has been established with an output ranging from 1.3 to 1.9 µm and few ps duration. The pump beam generation has been implemented based on rod-type fiber amplifiers producing more than 37 W average power and 370 kW peak power. The utility of this system as an OPCPA pump laser is presented along with the OPA design. The discussed systems operate in radically different regimes in terms of peak power, average power, and repetition rate. The anticipated OPCPA systems with few-cycle duration enable a wide range of novel experimental studies in attoscience, ultrafast materials processing, filamentation, LIBS and coherent control

Doctor of Philosophy / Department of Industrial & Manufacturing Systems Engineering / Shuting Lei / Lasers have been widely used as a manufacturing tool for material processing, such as drilling, cutting, welding and surface texturing. Compared to traditional manufacturing methods, laser-based material processing is high precision, can treat a wide range of materials, and has no tool wear. However, demanding manufacturing processes emerging from the needs of nano and 3D fabrication require the development of laser processing strategies that can address critical issues such as machining resolution, processing speed and product quality. This dissertation concerns the development of novel laser processing strategies based on spatial, temporal and spectral control of light-matter interaction. In the spatial domain, beam shaping is employed in ultrafast laser micro-processing. Zero-order Bessel beam, generated by an axicon, is used for selective removal of the back contact layer of thin film solar cells. Bessel beam’s propagation-invariance property gives rise to an extension of focal range by orders of magnitude compared to Gaussian beam, greatly increasing process tolerance to surface unevenness and positioning error. Together with the axicon, a spatial light modulator is subsequently used to modify the phase of laser beam and generate superpositions of high-order Bessel beam with high energy efficiency. With the superposed beam, processing speed can be increased significantly, and collateral damage resulting from the ring structures in the zero-order Bessel beam can be greatly suppressed. In the temporal domain, it is demonstrated that ionization in dielectric materials can be controlled with a pair of ultraviolet and infrared pulses. With the assistance of the long-wavelength infrared pulse, nano-scale features are achieved using only a small fraction of threshold energy for the short-wavelength pulse. Computer simulation based on the rate equation model is conducted and found to be in good agreement with experimental results. This study paves the way for future adoption of short-wavelength laser sources, for example in the extreme ultraviolet range, for direct laser nano-fabrication with below-threshold pulse energy. In the spectral domain, a short-wavelength infrared laser is used to generate modification in the bulk of silicon wafers, in an attempt to develop 3D fabrication capabilities in semiconductors. Issues such as spherical aberration correction and examination procedure are addressed. Permanent modification is generated inside silicon by tightly focusing and continuously scanning the laser beam inside the samples, without introducing surface damage. The effect of laser pulse energy and polarization is also investigated. These results demonstrate the potential of controlling laser processing in multiple dimensions for manufacturing purposes, and point to a future when laser can be used as naturally and efficiently as mechanical tools used today, but is targeted at more challenging problems.

In the past decade, ultrashort laser sources have had a decisive impact on material processing for photonic applications. The technique is usually restricted to the elemental association of an ultrashort source with a focusing lens. It is thus limited in the achievable bulk modifications. Accompanying studies of material modifications in space and time, we propose here that automated spatio-temporal tailoring of the laser pulses is an efficient manner to overcome these limitations. More precisely, we demonstrate the generation of multiple processing foci for synchronous photomachining of multiple devices in the bulk. Thus, we report on the parallel photowriting of waveguides, light couplers, light dividers in 2D/3D in fused silica glass. We show that the domain of photowriting can be extended to deep focusing. We indicate that this can be achieved by wavefront shaping or temporal profile tailoring conducted by an evolutionary optimization loop. We also have unveiled a singular interaction regime where regular structuring takes place before the focal region. For the first time, the dynamics of the energy coupling to the glassy matrix is evaluated for various temporal pulse profiles. Enhanced energy confinement in the case of picosecond pulses is confirmed by characterization of the transient electronic gas and of the subsequent pressure. These pump-probe studies were carried out with a self-build time-resolved microscopy system with temporally shaped pump irradiation. We also developed a new method based on the Drude model to differentiate the electronic and matrix contributions to the contrast of the microscopy images.

Metal halide perovskites have emerged as photoactive materials in solution-processed devices thanks to their unique properties such as high absorption coefficient, sharp absorption edge, long carrier diffusion lengths, and tunable bandgap, together with ease of fabrication. The single-junction perovskite solar cells have reached power conversion efficiencies of more than 25%. Although the efficiency of perovskite devices has increased tremendously in a very short time, the efficiency is still limited by carrier recombination at defects and interfaces. Thus, understanding these losses and how to reduce them is the way forward towards the Shockley-Queisser limit. This thesis aims to apply ultrafast optical spectroscopy techniques to investigate the recombination pathways in halide perovskites, and understand the charge extraction from perovskite to transport layers and nonradiative losses at the interface. The first part focuses on perovskite solar cells with planar n–i–p device architecture which offers significant advantages in terms of large scale processing, the potential use of flexible substrates, and applicability to tandems. In addition to the optimization of MAPbI3 solar cell fabrication using a modified sequential interdiffusion protocol, the photophysics of perovskites exposed to humid air and illumination are discussed. The MAPbI3 film processed with the addition of glycol ethers to the methylammonium iodide solution results in the control of PbI2 to perovskite conversion dynamics, thus enhanced morphology and crystallinity. For samples exposed to humid air and illumination, the formation of sub-bandgap states and increased trap-assisted recombination are observed, using highly-sensitive absorption and time-resolved photoluminescence measurements, respectively. It appears that such exposure primarily affects the perovskite surface. The second part discusses the hole extraction from Cs0.07Rb0.03FA0.765MA0.135PbI2.55Br0.45 to the polymeric hole transport layer and interfacial recombination using ultrafast transient absorption spectroscopy technique. To illustrate this, PDPP-3T was used as HTL, since its ground state absorption is red-shifted compared to the perovskite’s photobleach, thereby allowing direct probing of the interfacial hole extraction and recombination. Moreover, carrier diffusion is investigated by varying the perovskite film thickness, and carrier mobility is found to be 39 cm2V-1s-1. Finally, hole extraction is found to be one order of magnitude faster than the recombination at the interface.

No description available.

<p>This thesis presents investigations on ultrafast laser irradiation of silicon towards the goal of hybridizing ultrafast laser processing and conventional semiconductor fabrication techniques to improve device applications. The fundamental sub-threshold damage accumulation mechanisms for potential defect engineering applications were studied through the use of positron annihilation spectroscopy, in situ sample heating during laser irradiation, varying the laser repetition rate, and samples implanted with various ion species at different conditions. Positron annihilation spectroscopy results suggest an increase in the divacancy density at the surface region of silicon following near- and slightly sub-threshold ultrafast laser irradiations. Laser irradiations at increasing sample temperature up to 600°C show a general decreasing trend of single-shot thresholds, and an increase in the suppression of sub-threshold damage accumulation. There is also a temperature dependence on the surface morphology resulting from ultrafast laser irradiation. Ion implantation modified the ablation threshold fluence, and a dependence on the ion implantation conditions was observed. Surface microstructuring of silicon was shown to improve absorption of light with a sub-bandgap wavelength of 1550 nm. An initial attempt with sulfur implantation did not exhibit further improvement in the optical absorption, and first attempts in device fabrication did not provide photoresponsivity at sub-bandgap wavelengths. Ultrafast laser irradiation of SiO₂-on-Si structures yielded different modification thresholds for different thicknesses of the oxide layer. Surface morphologies obtained in the irradiation of these structures can affect potential applications. Selected studies of ultrafast laser irradiation of GaP, metal-SiO₂-Si structures, quartz, diamond, and porcine bone demonstrated similarities in ablation behavior and morphologies, and the potential for a broad range of applications. The results in combination with the proposed future work in this thesis can contribute to potential device applications while providing valuable insights into the ultrafast laser ablation mechanisms.</p> / Doctor of Philosophy (PhD)

This dissertation expounds growing insight of the electrospray droplet ionization mechanism following ablation of dried hydrophobic and hydrophilic molecules using femtosecond laser pulses and mass analysis of the gas phase ions. Both hydrophobic and hydrophilic molecules were laser vaporized into an electrospray solvent opposite in polarity revealing appreciable ion intensity for all samples in contrast to ESI-MS and DESI measurements were solubility of the analyte in the spray solvent is a prerequisite. Quantitative analysis of equimolar protein solutions was established using LEMS reporting over three decades of quantitave response with little evidence of ion suppression. In contrast, ESI-MS measurements of similar equimolar protein solutions revealed severe ion suppression eliminating ion current from one of the protein analytes. Finally, the nature of an analyte following nonresonant laser vaporization has been the subject of debate. Aqueous trypsin was laser vaporized into an electrospray solvent containing either buffer or acid with substrate. LEMS measurements using buffer revealed enzyme-substrate intermediate charge states and continued enzymatic activity while the lack of enzyme-substrate intermediates and stymied enzymatic activity observed using acid suggests nonresonant laser vaporization preserves solution phase structure. This dissertation also extends considerably the use of LEMS for identification and characterization of energetic materials in their pre- and post-blast forms without sample preparation. The use of mulivarate analysis for the classification of large sample sets was also demonstrated showing high fidelity assignment of commercial formulations to their manufacturer. Five unburnt smokeless powders investigated using LEMS revealed unique combinations of organic molecules such as stabilizers and plasticizers using a simple electrospray solvent. Principal component analysis (PCA) provided exact classification of the mass spectra with respect to the manufacturer of the ordinance. LEMS measurements were then obtained from five commercial gunshot residue samples, or post-blast smokeless powder, revealing trace amounts of organics such as the stabilizers and large quantities of inorganic barium originating from the primer. Principal component analysis (PCA) again provided exact classification of the gunshot residue mass spectra with respect to the manufacturer of the ordinance. The use of a common transition metal complexation agent enabled full characterization of eight gunshot residue samples to include the heavy metals contained in the primer and the organics such as the stabilizers and plasticizers without any sample preparation or pre-concentration procedures. Principal component analysis (PCA) again provided high fidelity classification of the gunshot residue mass spectra with respect to the manufacturer of the ordinance after mass analysis with LEMS. Finally, highly energetic formulations such as composition 4 (C-4) and detonation cord subjected to nonresonant femtosecond laser vaporization enabled full characterization of these complex compositions identifying binders, stabilizers, the explosive ingredient and age-related decomposition derivative signature molecules with appreciable ion current detected using both positive and negative ion modes. / Chemistry

This work is devoted to the investigation of a spin polarization in ferromagnetic semiconductor Ga1-xMnxAs with a broad nominal concentration of manganese ions using one method of the ultrafast laser spectroscopy - the time-resolved Kerr rotation. At first, the experimental setup was optimized for the investigation of the dynamics of spin polarized charge carriers in semiconductors which were photo-generated by circularly polarized laser pulses. It was observed that the measured signal is induced by spin-polarized electrons. Due to a small thickness of the investigated ferromagnetic films the measured signal probably monitored the dynamics of fotogenerated electrons in GaAs substrate. Nevertheless, the measured data show that the electron spin dynamics in the substrate is significantly influenced by proximity effect due to the deposited ferromagnetic layer.

Doctor of Philosophy / Department of Physics / Itzhak Ben-Itzhak / The use of ultrafast lasers allows one to study and even control quantum mechanical systems on their natural timescales. Our aim is to study the fragmentation of small molecules in strong laser fields as a means to gain understanding of molecular dynamics and light-matter interactions. Our research group has utilized fast, positively charged molecular ion beams as targets to study and control fragmentation by strong laser fields. This approach allows for detection of all molecular fragments including neutrals, and a coincidence three-dimensional momentum imaging technique is used to characterize the fragmentation. A natural extension of these types of studies is to expand the types of molecular systems that can be studied, from positively charged molecules to neutral and negatively charged molecules. To that end, the primary technical development of this dissertation involved the generation and use of fast, negatively charged molecular beams. Using fast molecular anion beams as targets allows for the study of fragmentation in which all fragments are neutral. As a demonstration, we employ this capability to study F2- dissociation and photodetachment. The dissociation pathways are identified and used to evaluate the initial vibrational population of the F2- beam. The role of dissociation in photodetachment is also explored, and we find that it competes with other dissociative (F+F) and non-dissociative (F2) photodetachment mechanisms. Also highlighted are studies of fragmentation of LiO-, in which the dissociation into Li+O- fragments provides information about the structure of Li O-, including the bond dissociation energy, which was found to be larger than values based on theory. Studies of the autodetachment lifetimes of Li O- were also performed using a pump-probe technique. Additional experimental advancements have made successful pump-probe studies of the ionization of HD+ and Ar2+ possible. Enhancement in the ionization of dissociating HD+ and Ar2+ was observed at surprisingly large internuclear separation where the fragments are expected to behave like separate atoms. The analysis methods used to quantify this enhancement are also described. Finally, the production of excited Rydberg D* fragments from D2 molecules was studied utilizing a state-selective detection method. The carrier-envelope phase dependence of D* formation was found to depend on the range of excited final states of the atomic fragments. We also measured the excited state population of the D* fragments. Together, the studies presented in this work provide new information about fragmentation of positive, negative, and neutral molecules in strong laser fields, and the experimental developments serve as building blocks for future studies that will lead to a better understanding of molecular dynamics.