We demonstrate experimentally that the multiphoton ionization rate in gallium arsenide depends on the alignment of the laser polarization with respect to the crystal axis. We show real-time modulation of 1900nm laser ionization rate, through viewing transmission, which mimics the symmetry of the semiconductor crystal. We propose that the modulation in the ionization rate arises because the varying reduced effective carrier mass, as predicted by Keldysh theory. We show direct comparison of the experimental transmission modulation depth with that predicted by Keldysh theory. This opens up a novel method for real-time non-invasive crystallography of crystalline materials.

Master of Science / Department of Physics / Itzhak Ben-Itzhak / Ultrafast lasers allow us to study molecular dynamics on their natural timescale. The electronic dynamics can be studied using attosecond pulses, while the vibrational and rotational dynamics can be probed using tens of femtosecond and picosecond laser pulses, respectively. This capability has led to a broad understanding of the electronic dynamics in atoms and molecules as well as vibrational and rotational dynamics of molecules, which is one of the important goals in basic science. Moreover, it is possible to control quantum mechanical processes using ultrafast intense lasers. In this thesis, we focus on a couple of experiments. The first involves quantum control of the formation of neutral molecular fragments while the second focuses on three-body fragmentation of molecules employing the native-frames analysis method, which was recently introduced by our group [J. Rajput et al., Phys. Rev. Lett. 120, 103001 (2018)]. Experimental studies focused on the formation of excited neutral D fragments from D2 molecules are presented. We show that by manipulating the chirp of the intense laser pulses, i.e. the “time order” of the frequency components within the pulse, the formation of these fragments is controlled. To achieve this control we implement a single-prism compressor to manipulate the chirp of the laser pulses. Three-body fragmentation of CO₂ resulting in C+ + O+ + O+ is also studied. We show that if the two bonds break in a two-step process, i.e. a sequential breakup, the pathways from which the two identical O+ fragments originate can be separated using the native-frames analysis method. In contrast, the two O+ fragments cannot be distinguished if the two C-O bonds break simultaneously.

We demonstrate experimentally that the multiphoton ionization rate in gallium arsenide depends on the alignment of the laser polarization with respect to the crystal axis. We show real-time modulation of 1900nm laser ionization rate, through viewing transmission, which mimics the symmetry of the semiconductor crystal. We propose that the modulation in the ionization rate arises because the varying reduced effective carrier mass, as predicted by Keldysh theory. We show direct comparison of the experimental transmission modulation depth with that predicted by Keldysh theory. This opens up a novel method for real-time non-invasive crystallography of crystalline materials.

We demonstrate experimentally that the multiphoton ionization rate in gallium arsenide depends on the alignment of the laser polarization with respect to the crystal axis. We show real-time modulation of 1900nm laser ionization rate, through viewing transmission, which mimics the symmetry of the semiconductor crystal. We propose that the modulation in the ionization rate arises because the varying reduced effective carrier mass, as predicted by Keldysh theory. We show direct comparison of the experimental transmission modulation depth with that predicted by Keldysh theory. This opens up a novel method for real-time non-invasive crystallography of crystalline materials.

No description available.

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.

Doctor of Philosophy / Department of Physics / Daniel Rolles / Modern laser sources can produce bursts of light that surpass even the fastest molecular vibrations. With durations this short even moderate pulse energies generate peak powers exceeding the average power output of the entire globe. When focused, this can result in an ultrafast electric field greater than the Coulomb potential that binds electrons to nuclei. This strong electric field strips electrons away from atoms in a process known as strong-field ionization. The first experimental realization of photoionization with intense laser pulses occurred only a few years after the invention of the laser. Yet, despite decades of intensive investigation, open questions remain. At the same time, the knowledge gained has led to the creation of multiple exciting fields such as attoscience, femtochemistry, and ultrafast nano-photonics. In this thesis I present my work to advance the fundamental understanding of intense, ultrafast light-matter interactions as well as efforts to expand the technological capabilities of ultrafast light sources and measurement techniques. This includes the photoionization pro- cess of atoms and nanoparticles subject to intense, mid-infrared laser fields. The resulting photoelectron emission is measured, with high precision, in a velocity map imaging spec- trometer. Other parts of this thesis detail my work on the generation and characterization of non-Gaussian optical pulses. Femtosecond Bessel beams are used to drive and study high harmonic generation with the ultimate goal of creating a compact, high-flux XUV source. Further studies include few-cycle pulses and the carrier-envelope phase, specifically methods of locking and tagging the carrier-envelope phase. A single-shot, all optical tagging method is developed and directly compared to the standard tagging method, the carrier-envelope phase meter. Finally, both experimental and computational studies are presented investigating the ultrafast thermal response cycle of nanowires undergoing femtosecond heating.

The generation of high-order harmonics opened an era of attosecond science wherein coherent light bursts are used to probe dynamic processes in matter with a time resolution short enough to resolve the motions of electrons. It enabled the development of extreme ultraviolet (XUV) and X-ray table-top sources with both temporal and spatial coherence, which provides the ability to shape the temporal and spatial structure of the XUV pulses. Scientists developed techniques to control and measure the temporal structure high harmonic emissions. These techniques exploited control of the driving laser pulse in the time domain and facilitated development of more advanced high-harmonic based XUV sources that have greatly impacted ultrafast measurements. In this thesis, I apply techniques to control and measure the spatial structure of high harmonic emissions, and discuss the underlying physics and potential applications of the interaction between spatially structured laser beams and materials. This study exploits the spatial degree of freedom in strong field interaction, which has not been given as much attention as the temporal degree of freedom. I use liquid crystal devices to shape the wave front of a fundamental laser beam to a vortex structure, then imprint this structured wave front onto XUV beams through high harmonic generation. This method provides an alternative to special XUV optics, which can manipulate the wave front of XUV radiation by all optical means. This result also reveals the conservation of orbital angular momentum in this extreme nonlinear wave mixing process. In addition to shaping the wave front, shaping the polarization of the driving beam also allows generation of circularly polarized the XUV radiation using a high harmonic source. This thesis also highlights the interplay between shaping the wave front and polarization in the high harmonic generation process. The topology of the structured beam can be maintained through this extreme nonlinear interaction due to the spin selection rules and spin-orbit conservation. Moreover, this thesis demonstrates an approach to integrate a vector beam into a broadband ultrafast light source and overcome the bandwidth limitation of mode converters. We use this approach to generate a few-cycle structured beam. In the future, this beam will be used to generate a strong ultrafast magnetic impulse in gas and solid targets by driving currents in a loop, which is a valuable tool for the future of magnetic metrology. The novel properties of structured laser beams discussed in this thesis expanded the capabilities of high harmonic based XUV sources and have opened a new field to explore this additional degree of freedom in strong field interactions.

The adiabatic approximation is a natural approach for the description of phenomena induced by low frequency laser radiation because the ratio of the laser frequency to the characteristic frequency of an atom or a molecule is a small parameter. Since the main aim of this work is the study of ionization phenomena, the version of the adiabatic approximation that can account for the transition from a bound state to the continuum must be employed. Despite much work in this topic, a universally accepted adiabatic approach of bound-free transitions is lacking. Hence, based on Savichev's modified adiabatic approximation [Sov. Phys. JETP 73, 803 (1991)], we first of all derive the most convenient form of the adiabatic approximation for the problems at hand. Connections of the obtained result with the quasiclassical approximation and other previous investigations are discussed. Then, such an adiabatic approximation is applied to single-electron ionization and non-sequential double ionization of atoms in a strong low frequency laser field. The momentum distribution of photoelectrons induced by single-electron ionization is obtained analytically without any assumptions on the momentum of the electrons. Previous known results are derived as special cases of this general momentum distribution. The correlated momentum distribution of two-electrons due to non-sequential double ionization of atoms is calculated semi-analytically. We focus on the deeply quantum regime -- the below intensity threshold regime, where the energy of the active electron driven by the laser field is insufficient to collisionally ionize the parent ion, and the assistance of the laser field is required to create a doubly charged ion. A special attention is paid to the role of Coulomb interactions in the process. The signatures of electron-electron repulsion, electron-core attraction, and electron-laser interaction are identified. The results are compared with available experimental data. Two-electron correlated spectra of non-sequential double ionization below intensity threshold are known to exhibit back-to-back scattering of the electrons, viz., the anticorrelation of the electrons. Currently, the widely accepted interpretation of the anticorrelation is recollision-induced excitation of the ion plus subsequent field ionization of the second electron. We argue that there exists another mechanism, namely simultaneous electron emission, when the time of return of the rescattered electron is equal to the time of liberation of the bounded electron (the ion has no time for excitation), that can also explain the anticorrelation of the electrons in the deep below intensity threshold regime. Finally, we study single-electron molecular ionization. Based on the geometrical approach to tunnelling by P. D. Hislop and I. M. Sigal [Memoir. AMS 78, No. 399 (1989)], we introduce the concept of a leading tunnelling trajectory. It is then proven that leading tunnelling trajectories for single active electron models of molecular tunnelling ionization (i.e., theories where a molecular potential is modelled by a single-electron multi-centre potential) are linear in the case of short range interactions and ``almost'' linear in the case of long range interactions. The results are presented on both the formal and physically intuitive levels. Physical implications of the proven statements are discussed.

The adiabatic approximation is a natural approach for the description of phenomena induced by low frequency laser radiation because the ratio of the laser frequency to the characteristic frequency of an atom or a molecule is a small parameter. Since the main aim of this work is the study of ionization phenomena, the version of the adiabatic approximation that can account for the transition from a bound state to the continuum must be employed. Despite much work in this topic, a universally accepted adiabatic approach of bound-free transitions is lacking. Hence, based on Savichev's modified adiabatic approximation [Sov. Phys. JETP 73, 803 (1991)], we first of all derive the most convenient form of the adiabatic approximation for the problems at hand. Connections of the obtained result with the quasiclassical approximation and other previous investigations are discussed. Then, such an adiabatic approximation is applied to single-electron ionization and non-sequential double ionization of atoms in a strong low frequency laser field. The momentum distribution of photoelectrons induced by single-electron ionization is obtained analytically without any assumptions on the momentum of the electrons. Previous known results are derived as special cases of this general momentum distribution. The correlated momentum distribution of two-electrons due to non-sequential double ionization of atoms is calculated semi-analytically. We focus on the deeply quantum regime -- the below intensity threshold regime, where the energy of the active electron driven by the laser field is insufficient to collisionally ionize the parent ion, and the assistance of the laser field is required to create a doubly charged ion. A special attention is paid to the role of Coulomb interactions in the process. The signatures of electron-electron repulsion, electron-core attraction, and electron-laser interaction are identified. The results are compared with available experimental data. Two-electron correlated spectra of non-sequential double ionization below intensity threshold are known to exhibit back-to-back scattering of the electrons, viz., the anticorrelation of the electrons. Currently, the widely accepted interpretation of the anticorrelation is recollision-induced excitation of the ion plus subsequent field ionization of the second electron. We argue that there exists another mechanism, namely simultaneous electron emission, when the time of return of the rescattered electron is equal to the time of liberation of the bounded electron (the ion has no time for excitation), that can also explain the anticorrelation of the electrons in the deep below intensity threshold regime. Finally, we study single-electron molecular ionization. Based on the geometrical approach to tunnelling by P. D. Hislop and I. M. Sigal [Memoir. AMS 78, No. 399 (1989)], we introduce the concept of a leading tunnelling trajectory. It is then proven that leading tunnelling trajectories for single active electron models of molecular tunnelling ionization (i.e., theories where a molecular potential is modelled by a single-electron multi-centre potential) are linear in the case of short range interactions and ``almost'' linear in the case of long range interactions. The results are presented on both the formal and physically intuitive levels. Physical implications of the proven statements are discussed.