Doctor of Philosophy / Department of Physics / Charles L. Cocke / The broad objective of ultrafast strong-field studies is to be able to measure and control atomic and molecular dynamics on a femtosecond timescale. This thesis work has two major themes: (1) Study of high-energy photoelectron distributions from atomic targets. (2) Electron localization control in atomic and molecular reactions using shaped laser pulses. The first section focuses on the study of photoelectron diffraction patterns of simple atomic targets to understand the target structure. We measure the full vector momentum spectra of high energy photoelectrons from atomic targets (Xe, Ar and Kr) generated by intense laser pulses. The target dependence of the angular distribution of the highest energy photoelectrons as predicted by Quantitative Rescattering Theory (QRS) is explored. More recent developments show target structure information can be retrieved from photoelectrons over a range of energies, from 4U$_p$ up to 10U$_p$, independent of the peak intensity at which the photoelectron spectra have been measured. Controlling the fragmentation pathways by manipulating the pulse shape is another major theme of ultrafast science today. In the second section we study the asymmetry of electron (and ion) emission from atoms (and molecules) by interaction with asymmetric pulses formed by the superposition of two colors (800 $\&$ 400 nm). Xe electron momentum spectra obtained as a function of the two-color phase exhibit a pronounced asymmetry. Using QRS theory we can analyze this asymmetric yield of the high energy photoelectrons to determine accurately the laser peak intensity and the absolute phase of the two-color electric field. This can be used as a standard pulse calibration method for all two-color studies. Experiments showing strong left-right asymmetry in D$^+$ ion yield from D$_2$ molecules using two-color pulses is also investigated. The asymmetry effect is found to be very ion-energy dependent.

Doctor of Philosophy / Department of Physics / Brett D. DePaola / In recent years, advance in ultra fast lasers and related optical technology has enhanced the ability to control the interaction between light and matter. In this dissertation, we try to improve our understanding of the interaction of atomic and molecular ladder systems with short optical pulses. A train of pulses produced by shaping the spectral phase of a single pulse from an ultra fast laser allows us to control the step-wise excitation in rubidium (Rb) atoms. As a diagnostic method, we use magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) to prepare cold target atoms and to observe atomic ions as a result of the interaction. We have explored the interactions of a finite number of optical short pulses in a train with a three-level Rb atom ladder system. Each pulse in the train is separated by a constant time interval with a fixed pulse-to-pulse phase change. In these experiments, two dimensional (2D) landscape maps show the interaction by measuring population in the uppermost state of the ladder system as a function of pulse-to-pulse time interval and phase shift. The observed structures in the 2D landscape are due to constructive or destructive interference in the interaction. Furthermore, different numbers of pulses in the train are applied to the atomic Rb three level ladder system in order to measure the effect on the interaction. The sharpness of the interference structure is enhanced by increasing the number of pulses. This phenomenon is analogous to increasing the sharpness in an optical multi-slit experiment by increasing the number of slits.

Master of Science / Department of Physics / Brett D. DePaola / A recent powerful spectroscopic technique that has been implemented using femtosecond lasers excites atoms or molecules through quantum interference effects. The results are oscillations in excited state populations that represent the optical frequencies used in the excitation pathway, these frequencies can be found by Fourier analysis. The technique uses a Mach-Zender interferometer wherein one femtosecond pulse is split into two pulses that are phase coherent. These pulses are the pump and probe pulses which are delayed with respect to one another by a variable time. During the delay between pulses the state excited by the first (pump) pulse evolves in time before the probe pulse is used to excite the atom into its final state. The observed final state population exhibits interference between the several possible pathways to the final state. The information gained from this method will allow for advances in other processes such as the dynamics of photo-association.

Master of Science / Department of Physics / Uwe Thumm / In this work we studied the dynamics of deuterium molecules in intense laser fields both experimentally and theoretically. For studying the dynamics of the molecule on a time scale that is less than the period of the laser field (2.7 fs for 800 nm), an advanced experimental technique: COLTRIMS (cold target recoil ion momentum spectroscopy) was used. COLTRIMS allows studying the nuclear dynamics without using attosecond laser pulses. This thesis consists of two main parts. In the first part we deduced the angular dependence of the ionization probability of the molecule without aligning the molecules, by measuring the relative angle between a deuteron resulting from field dissociation and an emitted electron using electron-ion coincidence measurements with circularly polarized light in COLTRIMS. We found out that for 50 fs pulses (1850 nm wavelength and 2 x10[superscript]14 W/cm[superscript]2 intensity), D[subscript]2 molecules are 1.15 times more likely to be ionized when the laser field is parallel to the molecular axis than when the laser field is perpendicular. This result agreed perfectly with the result from our ab initio theoretical model and also with predictions of the molecular Ammosov-Delone-Krainov (mo-ADK) theory. In the second part of this work we calculated the time evolution of an initial nuclear wave packet in D[subscript]2[superscript]+ generated by the rapid ionization of D[subscript]2 by an ultra short laser pulse. We Fourier transformed the nuclear probability density with respect to the delay between the pump and probe pulses and obtained two-dimensional internuclear-distance-dependent power spectra which serve as a tool for visualizing and analyzing the nuclear dynamics in D[subscript]2[superscript]+ in an external laser field. We attempt to model realistic laser pulses, therefore in addition to the main spike of the pulse we include the Gaussian pedestal. The optimal laser parameters for observing field-induced bond softening and bond hardening in D[subscript]2[superscript]+ can be achieved by varying the intensity, wavelength, and duration of the probe-pulse pedestal. Despite the implicit “continuum wave” (infinite pulse length) assumption the validity of the “Floquet picture” is tested for the interpretation of short-pulse laser-molecule interactions.

Doctor of Philosophy / Department of Physics / Igor V. Litvinyuk / The goal of this dissertation project was to study the dynamics of nuclear motion in diatomic (H[subscript]2, N[subscript]2, O[subscript]2, CO) and triatomic (CO[subscript]2) molecules initiated by the ionization and/or excitation of these molecules with near-IR few-cycle laser pulses. This dynamics includes vibrational and rotational motion on the electronic potential surfaces of the molecules and their molecular ions. The experimental techniques used included the pump-probe approach, laser Coulomb explosion imaging and the COLTRIMS technique. The results are presented in four chapters. A study of rotational and vibrational nuclear dynamics in H[subscript]2 and D[subscript]2 molecules and ions initiated by 8 fs near-IR pulses is presented in Chapter 4. Transient alignment of the neutral molecules was observed and simulated; rotational frequency components contributing to the rotational wavepacket dynamics were recovered. Chapter 5 is dedicated to revealing the contribution of excited dissociative states of D[subscript]2[superscript]+ ions to the process of fragmentation by electron recollision. It was shown that it is possible to isolate the process of resonant excitation and estimate the individual contributions of the [superscript]2sigma[subscript]u[superscript]+ and [superscript]2pi[subscript]u states. In Chapter 6 the subject of investigation is the nuclear dynamics of N[subscript]2, O[subscript]2 and CO molecules initiated by ionization of a neutral molecule by a short intense laser pulse. It was shown that the kinetic energy release of the Coulomb explosion fragments, measured as a function of the delay time between pump and probe pulses, reveals the behavior of nuclear wave packet evolution on electronic states of the molecular ions. It was shown that information on the dissociation and excitation pathways can be extracted from the experimental spectra and the relative contributions of particular electronic states can be estimated. Chapter 7 is focused on studying the fragmentation of CO[subscript]2 following the interaction of this molecule with the laser field. The most important result of this study was that it presented direct experimental evidence of charge-resonant enhanced ionization (CREI), a phenomenon well-studied for diatomic molecules and predicted theoretically for triatomic molecules. The critical internuclear distance, the relevant ionic charge state and a pair of charge-resonant states responsible for the CREI were also found.

Doctor of Philosophy / Department of Physics / Zenghu Chang / The observation and control of dynamics in atomic and molecular targets requires the use of laser pulses with duration less than the characteristic timescale of the process which is to be manipulated. For electron dynamics, this time scale is on the order of attoseconds where 1 attosecond = 10[superscript]-18 seconds. In order to generate pulses on this time scale, different gating methods have been proposed. The idea is to extract or “gate” a single pulse from an attosecond pulse train and switch off all the other pulses. While previous methods have had some success, they are very difficult to implement and so far very few labs have access to these unique light sources. The purpose of this work is to introduce a new method, called double optical gating (DOG), and to demonstrate its effectiveness at generating high contrast single isolated attosecond pulses from multi-cycle lasers. First, the method is described in detail and is investigated in the spectral domain. The resulting attosecond pulses produced are then temporally characterized through attosecond streaking. A second method of gating, called generalized double optical gating (GDOG), is also introduced. This method allows attosecond pulse generation directly from a carrier-envelope phase un-stabilized laser system for the first time. Next the methods of DOG and GDOG are implemented in attosecond applications like high flux pulses and extreme broadband spectrum generation. Finally, the attosecond pulses themselves are used in experiments. First, an attosecond/femtosecond cross correlation is used for characterization of spatial and temporal properties of femtosecond pulses. Then, an attosecond pump, femtosecond probe experiment is conducted to observe and control electron dynamics in helium for the first time.

Doctor of Philosophy / Department of Physics / Brett D. DePaola / In many experiments involving a magneto-optical trap (MOT) it is of great importance to know the fraction of atoms left in an excited state due to the trapping process. Generally speaking, researchers have had to use overly simplistic and untested models to estimate this fraction. In this work, the excited fraction of 87Rb atoms in a MOT is measured using a model-free approach. A simple model is fit to the fractions which were obtained for a range of MOT parameters. Using the results of this work, the excited fraction of 87Rb atoms trapped in a MOT can be accurately estimated with knowledge of only the trapping laser intensity and detuning. The results are only weakly dependent on other MOT parameters.

Doctor of Philosophy / Department of Physics / Zenghu Chang / It is still a dream to image the dynamics of electrons in atoms and molecules experimentally. This is due to the fact that such motion takes place in an ultra-short time scale; for example, an electron moves around the Bohr orbit in about 150-as (1 as = 10 -18 s), and pulses much shorter than this limit are not currently available to probe such fast dynamics. In recent years, an isolated single attosecond pulse has been produced by extracting the cutoff of harmonic spectrum driven by a laser pulse as short as ~ 5fs (1fs =10-15 s). But, these pulses are still too long in order to make the dream come true. Here, we study the possibility of generation of a much shorter and wavelength tunable single attosecond pulse by using polarization gating. In the experiment, we compressed ~30fs pulses from the laser amplifier down to ~6fs and characterized them. These linearly polarized pulses were converted to ellipticity varying pulses, and by exploiting the property of the strong dependence of the harmonic signal with the ellipticity of the laser, an XUV supercontinuum was produced in the harmonic spectrum which could support 60-as pulses. The bandwidth of such a supercontinuum, and therefore the duration of the attosecond pulses, is limited mainly by the currently available energy of the driving laser pulses at few cycle limits. In this project, we present an approach which allowed us to scale up the energy of such pulses by a factor of 1.5 in “Hollow Core Fiber / Chirped Mirrors Compressor”. Finally, in order to temporarily characterize the attosecond pulses we designed and built an “Attosecond Streak Camera”. Most of such cameras to date are limited to measuring a 1 dimensional energy spectrum and have only a few degrees of acceptance angle. Our camera is capable of measuring 2d momentum of the photoelectrons with large acceptance angle, for example ~ 65o at the photoelectron of energy ~15 eV. Recently, we observed the sidebands in addition to the main peaks in their laser assisted XUV photoelectron spectrum. The single attosecond pulses, after being characterized with this high speed camera, can be used to explore the dynamics of electrons at the attosecond scale.

Doctor of Philosophy / Department of Physics / Brett D. DePaola / Many people in the science community are interested in the prospect of cold molecules for such applications as quantum computing and molecular Bose-Einstein condensates. Current methods of production fall short of the requirements for such projects. Photo association is a promising technique for forming cold molecules, but is currently facing significant obstacles. By understanding the photo association process and utilizing higher excited states, it is hoped that cold molecules can be formed from more easily produced cold atoms. Photo associative Ionization (PAI) is presented as a means to study excited state molecular dynamics at large internuclear separation, including photo association. This thesis presents a number of techniques for studying PAI in cold rubidium and a number of results obtained with the techniques. Excitation pathways for the process are explored in both narrow linewidth (MHz) and ultrafast (fs), large bandwidth (20 nm) domains.

Doctor of Philosophy / Department of Physics / Zenghu Chang / The few-cycle femtosecond laser pulse has proved itself to be a powerful tool for controlling the electron dynamics inside atoms and molecules. By applying such few-cycle pulses as a driving field, single isolated attosecond pulses can be produced through the high-order harmonic generation process, which provide a novel tool for capturing the real time electron motion. The first part of the thesis is devoted to the state of the art few-cycle near infrared (NIR) laser pulse development, which includes absolute phase control (carrier-envelope phase stabilization), amplitude control (power stabilization), and relative phase control (pulse compression and shaping). Then the double optical gating (DOG) method for generating single attosecond pulses and the attosecond streaking experiment for characterizing such pulses are presented. Various experimental limitations in the attosecond streaking measurement are illustrated through simulation. Finally by using the single attosecond pulses generated by DOG, an attosecond transient absorption experiment is performed to study the autoionization process of argon. When the delay between a few-cycle NIR pulse and a single attosecond XUV pulse is scanned, the Fano resonance shapes of the argon autoionizing states are modified by the NIR pulse, which shows the direct observation and control of electron-electron correlation in the temporal domain.