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 / Brett D. Esry / The nuclear rotational period of the simplest molecule H[subscript]2[superscript]+ is about 550 fs, which is more than 35 times longer than its vibrational period of 15 fs. The rotational time scale is also much longer than widely available ultra short laser pulses which have 10 fs or less duration. The large difference in rotational period and ultra short laser pulse duration raises questions about the importance of nuclear rotation in theoretical studies of H[subscript]2[superscript]+ dissociation by these pulses. In most studies, reduced-dimensionality calculations are performed by freezing the molecular axis in one direction, referred to as the aligned model. We have systematically compared the aligned model with our full-dimensionality results for total dissociation probability and field-free dynamics of the dissociating fragments. The agreement between the two is only qualitative even for ultra short 10 fs pulses. Post-pulse dynamics of the bound wave function show rotational revivals. Significant alignment of H[subscript]2[superscript]+ occurs at these revivals. Our theoretical formulation to solve the time-dependent Schrodinger equation is an important step forward to make quantitative comparison between theory and experiment. We accurately calculate observables such as kinetic energy, angular, and momentum distributions. Reduced-dimensionality calculations cannot predict momentum distributions. Our theoretical approach presents the first momentum distribution of H[subscript]2[superscript]+ dissociation by few cycle laser pulses. These observables can be directly compared to the experiment. After taking into account averaging steps over the experimental conditions, we find remarkable agreement between the theory and experiment. Thus, our theoretical formulation can make predictions. In H[subscript]2[superscript]+ dissociation by pulses less than 10 fs, an asymmetry in the momentum distribution occurs by the interference of different pathways contributing to the same energy. The asymmetry, however, becomes negligible after averaging over experimental conditions. In a proposed pump-probe scheme, we predict an order of magnitude enhancement in the asymmetry and are optimistic that it can be observed.

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.