Master of Science / Department of Physics / Brett D. Esry / The two-state field-aligned (1-D) model has been employed to investigate the dissociation dynamics of a hydrogen molecular ion and its isotopes under the Born-Oppenheimer approximation without rotation. The emphasis of this work was on the role of mass during the dynamical dissociation processes and on the laser-induced branching ratios between different photon pathways. Firstly, we have found that scaling the pulse duration of the laser pulse, applied to H[subscript]2+ and D[subscript]2+ , by the square root of the mass ratio of these isotopes will produce similar structure in the nuclear kinetic energy release (KER) spectra. In fact, the similarity of the spectra is enhanced by including some averaging that is necessary for comparison with experiment. For this to occur, the same broad initial vibrational distribution and a short pulse are preferred. Using this scaling idea, it is possible to produce effectively shorter laser pulses by studying heavier isotopes, like D[subscript]2+. Secondly, we have demonstrated analytically and numerically that there is a carrier-envelope phase effect in the total dissociation probability (TDP) of H[subscript]2+, and this effect grows with nuclear mass. We further show that under the same laser conditions, the CEP effect in the asymmetry between breakup channels decreases with mass. Our analytic expressions enhance the idea that CEP effects can be understood as an interference between different n-photon processes. Thirdly, the trends in the dissociation dynamics of H[subscript]2+ and D[subscript]2+ in a 800nm ultra short intense laser field were demonstrated by studying the dissociation branching ratios of multiphoton processes as a function of the laser peak intensity (from 8[times]10[superscript]9 to 10[superscript]14 W/cm[superscript]2) or pulse length (5fs-7.5fs). Based on the two-state approximation, an energy-analysis method (EAM) was employed to separate multiphoton processes. The results show that the one-photon dissociation process dominates over all other photon processes under all the laser conditions applied in the calculations and that the zero-photon process contributes to a surprisingly large fraction of the total dissociation. Two- and three- photon dissociation are weaker processes, but become more and more important as the laser peak intensity and pulse length increases. A two-state Floquet method was used to check the accuracy of the EAM, and good agreement between the two methods was found, demonstrating the reliability of the EAM. In comparison with H[subscript]2+, D[subscript]2+ displays stronger two and three photon branching ratios (above-threshold dissociation - ATD), which can be attributed to the late arrival of D[subscript]2+ to the critical distance for ATD to occur due to its heavier mass. Therefore, this "mass" effect can be used to steer the molecular dissociation pathways.

Doctor of Philosophy / Department of Physics / B.D. DePaola / In recent years, coherent excitation techniques have focused on the ability to efficiently prepare atomic or molecular systems into a selected state. Such population control plays a key role in cutting-edge research taking place today, such as in the areas of quantum information and laser-controlled chemical reactions. Stimulated Raman adiabatic passage (STIRAP) is a widely-used coherent excitation technique that provides a relatively robust control mechanism for efficiently exciting a target population into a desired state. While the technique is well proven, current experimental techniques yield little information on the population dynamics taking place throughout the excitation process, and experimentalists rely solely on final excited-state measurements to determine the efficiency of population transfer. This dissertation presents a unique diagnostic tool to measure multilevel coherent population transfer on a short (nanosecond) timescale. The technique described here uses magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) as a noninvasive probe of a coherently-controlled system. It provides extremely detailed information about the excitation process, and highlights some important characteristics seen in excited populations that would otherwise be misleading or completely overlooked if one were to use more traditional diagnostic techniques. This dissertation discusses both the theoretical and experimental results applied to three-level coherently excited target populations of Rb-87.

Master of Science / Department of Physics / Kristan L. Corwin / We investigate the nonlinear spectroscopy of acetylene in the near infrared region inside a photonic band gap fiber. The near infrared region of the optical spectrum is an area of intensive research due to its relevance to telecommunication and optical metrology. Acetylene provides a large number of reference transitions coincident with the international telecommunication band. Acetylene contains about 50 strong lines between 1510 nm and 1540 nm in the ν1+ν3 ro-vibrational combination band. We have observed the Doppler-free saturated spectrum of several of these lines. The light from a tunable diode laser at ~1531 nm, resonant with the P(11) transition, is amplified by an erbium doped fiber amplifier and split into a strong pump beam and weak probe beam which counter-propagate inside the gas-filled fiber. The measured Doppler linewidth of the P(11) line at room temperature is about 467 MHz wide. The sub-Doppler profile over a pressure range of 200-1600 mT appears as a narrow absorption feature about 20-40 MHz wide, even at the low pump power of ~10 mW. It is found that for a fiber with an 80 cm length, 20 core size, pumped with 29 mw, the optimum pressure is ~530mT. But the optimum pressure condition will further decrease when the fiber length increases.

Master of Science / Department of Mechanical and Nuclear Engineering / Steven J. Eckels / Christopher M. Sorensen / Large specific surface areas and high concentrations of reactive edge and defect sites make NanoActive™ metal oxide powders ideal chemical adsorbents. These powders are dispersed in aerosol form to remediate toxic wastes and neutralize chemical and biological warfare agents. In the destructive adsorption of toxic chemicals, effective application requires particles be as small as possible, thus, maximizing surface area and number of edge and defect sites. Other applications, e.g. smoke clearing, require particles be large so they will settle in a timely manner. Ideally, particle size control could be engineered into powder dispersion devices. The purpose of this study was to explore particle cohesion and aerodynamic deaggregation mechanisms to enhance the design of powder dispersion devices. An aerosol generator and four experimental nozzles were designed to explore the most commonly referenced deaggregation mechanisms: particle acceleration, particles in shear and turbulent flows, and particle impaction. The powders were then dispersed through the nozzles with increasing flow rates. A small angle light scattering device was used to make in situ particle size measurements. The nozzle designed for impaction deaggregated the NanoActive™ MgO particles to a lesser degree than the other three nozzles, which deaggregated the particles to a similar degree. Flows in three of the four nozzles were simulated in a commercial computational fluid dynamics package. Theoretical particle and aggregate stresses from the literature were calculated using simulated data. These calculations suggest particle acceleration causes internal stresses roughly three orders of magnitude larger than shear and turbulent flows. These calculations, coupled with experimental data, lead to the conclusion that acceleration was the most significant cause of particle deaggregation in these experiments. Experimental data also identified the dependence of deaggregation on primary particle size and agglomerate structure. NanoActive™ powders with smaller primary particles exhibited higher resistance to deaggregation. Small primary particle size was thought to increase the magnitude of van der Waals interactions. These interactions were modeled and compared to theoretical deaggregation stresses previously mentioned. In conclusion, deaggregation is possible. However, the ideas of particle size control and a universal dispersion device seem elusive considering the material dependent nature of deaggregation.

Doctor of Philosophy / Department of Physics / Uwe Thumm / The time-dependent Schrödinger equation is integrated on a numerical lattice for up to three-dimensional problems. The wave packet propagation technique has been applied to ion – atom collisions in a strong laser field, the vibrational nuclear motion in small homonuclear diatomic molecular ions, and for the scattering of an ion in front of a metallic surface. For laser-assisted proton – hydrogen collisions it is shown, that strong circularly polarized radiation significantly alters the capture and ionization probabilities and results in a dichroism with respect to the helicity. In a pump – control – probe scheme, “stroboscopic” exposure of a nuclear wave packet of the deuterium molecular ion by a single or a series of short and intense laser control pulses may be used to produce an almost stationary distribution of a single vibrational level, where the nodal structure can be tested using the Coulomb explosion imaging technique. Using a pump – probe setup with variable probe delays it is proposed to use Fourier analysis of the time dependence of the Coulomb explosion kinetic energy release spectrum to reveal insight into the initial vibrational state distribution for small diatomic molecules. A last application demonstrates, that resonant charge transfer for scattering of a negative hydrogen anion on a metal surface depends crucially on the position of surface and image states relative to the conduction and valence band, thereby implying different reaction mechanisms for different surface cuts of a metal.

Doctor of Philosophy / Department of Physics / Zenghu Chang / The first part of this thesis describes our novel design, test, and application of our X-ray streak camera to the pulse duration measurement of soft X-rays. We demonstrated a significant improvement in the resolution of the x-ray streak camera by reducing the electron beam size in the deflection plates. This was accomplished by adding a slit in front of the focusing lens and the deflection plates. The temporal resolution reached 280 fs when the slit width was 5 μm. The camera was operated in an accumulative mode and tested by using a 25 fs laser with 2 kHz repetition rate and 1-2% RMS pulse energy stability. We conclude that deflection aberrations, which limit the resolution of the camera, can be appreciably reduced by eliminating the wide-angle electrons. We also employed the same streak camera to demonstrate that it is capable of measuring the pulse duration of X-rays. We measured the pulse duration of X-rays emitted from Ni-like Ag and Cd grazing-incidence laser to be ~5ps. The measured value agrees with the prediction made by the model and the measurement made by changing the delay as a function of the pulse duration. The streak camera was also tested with various sources of X-ray such as high harmonics generation of soft x-rays from an argon atom using a high power Ti:sapphire laser source of KLS. The result of the measurement manifests its capability for serving as a detector in the study of ultrafast dynamics in the field of physics, chemistry, biology and medical sciences. The second part of this thesis describes our design of a spectrometer to study the effect of the Carrier envelope (CE) phase on polarization gated extreme-ultraviolet (XUV) super-continuum generation. Because the challenge of making single shot experiment possible is to generate a sufficient number of photons, our setup has been built to allow generation of high order harmonics at the maximum phase matched pressure. This is the first time to our knowledge that phase matching in the polarization gating process has been studied so far. We measured the maximum phase matching pressure to be ~ 55 Torr which is the pressure above which quadratic increase in intensity of the high harmonics spectrum ceases to appear. At this pressure the number of photons per laser shot was 104 which is sufficient for measuring the single shot XUV spectrum in the range 34 to 45 eV. The spectral profile was a super-continuum for some shots and discrete high harmonics for other shots. It is believed that the shot to shot variation of the spectra is due to the changes of the carrier envelope phase of the few-cycle laser pulses used for the polarization gating. An improved CE phase stabilization system in KLS further eliminated the statistical noise in our observation by allowing us to integrate data over several laser cycles for each CE phase value. The effect of CE phase on a polarization gated XUV spectrum was tested by changing the CE phase with two different methods. In the first method, the CE phase was changed by changing the thickness of fused silica plates on the beam path, and the result shows the shift in the spectral peak of the XUV when the gate width approached less than one optical cycle. As gate width was made less than half the optical cycle, the spectrum was observed with continuum harmonics separated by π radians. We believe that the presence of continuum and discrete harmonics spectra in the observation is due to single and double attosecond pulses generated in the polarization gating. In the second method the carrier-envelope phase of pulses from a grating-based chirped pulse amplification laser was varied smoothly to cover a 2π range by controlling the grating separation. The phase is measured simultaneously by an f-to-2f setup and by the variation of XUV spectra from polarization gated high harmonic generation. A very good similarity between the effect of single and double slits in Yong’s experiment and that of CE phase on the XUV spectrum in the polarization gating experiment has been found, giving better agreement with the theory. The effect of optical properties such as the Gouy phase shift on the polarization gated spectrum has also been studied in the course of investigating the best experimental optimizations to generate the most CE phase sensitive XUV spectrum with less statistical noise. This is the first time to our knowledge experimental study of the effect of the Gouy phase shift on a polarization gated XUV spectrum has been made.