Thesis (Ph.D.). / Written for the Dept. of Physics. Title from title page of PDF (viewed 2008/05/09). Includes bibliographical references.

Thesis (Ph.D.). / Written for the Dept. of Mining and Materials Engineering. Title from title page of PDF (viewed 2008/01/12). Includes bibliographical references.

Thesis (Ph. D.)--University of Washington, 1999. / Vita. Includes bibliographical references (leaves [74]-85).

Thesis (M. Phil.)--University of Hong Kong, 1994. / Includes bibliographical references.

Thesis (Ph. D.)--University of Wisconsin--Madison, 1974. / Typescript. Vita. Includes bibliographical references.

Thesis (Ph. D.)--University of Chicago, Dept. of Astronomy and Astrophysics. / Includes bibliographical references. Also available on the Internet.

Thesis (M.S.)--University of Missouri-Columbia, 2005. / The entire dissertation/thesis text is included in the research.pdf file; the official abstract appears in the short.pdf file (which also appears in the research.pdf); a non-technical general description, or public abstract, appears in the public.pdf file. Title from title screen of research.pdf file viewed on (December 18, 2006) Includes bibliographical references.

In 1915, Debye derived his well-known equation for the X-ray scattering from a sample of randomly orientated gas-phase molecules. He approximated the molecular scattering by adding the contributions of isolated atomic constituents. This is known as the Independent Atom Model (IAM). However, it omits the redistribution of valence electrons due to bonding, and is limited to the electronic ground state. The main proposition of this thesis is that it is worthwhile going beyond the IAM when interpreting X-ray scattering data. In part, this is motivated by the arrival of new X-ray sources called X-ray Free-Electron Lasers (XFELs). A new method called Ab Initio X-ray Diffraction (AIXRD) is introduced. It calculates the elastic X-ray molecular scattering factor directly from wave functions calculated by ab initio electronic structure theory, for instance Hartree-Fock or multiconfigurational self-consistent field. In this way, the valence electrons are correctly taken into account, and calculations based on electronically excited wave functions become possible. The wave functions must be constructed from spatial orbitals made up of Gaussian-Type Orbitals (GTOs), giving an analytical solution to the Fourier transform integrals involved, and is key to computationally efficient and accurate results. This is compared to a fast Fourier transform (FFT) method, where the electron density is computed on a 3D grid and an FFT algorithm is used to obtain the elastic X-ray molecular scattering factor. Inspired by post-crystallography experiments such as serial femtosecond crystallography and single-particle imaging at XFELs, the AIXRD method is expanded to allow accurate X-ray diffraction calculations from large molecules such as proteins. To make the underlying ab initio problem tractable, the molecule is split into fragments. In other words, the electron density is constructed by a sum of fragment contributions, as is the corresponding molecular form-factor. In this way, it is analogous to the IAM approach except that instead of isolated atoms, there are isolated fragments. A pairwise summation of fragment contributions is also used to account for fragment-fragment interactions. Various fragment definitions are compared based on their effect on the X-ray diffraction signal, and are compared to the IAM method. Finally, X-ray diffraction from molecules in specific quantum states is calculated, revealing a distinct quantum fingerprint in the X-ray diffraction, and a comparison to experiment is made. In particular, the elastic X-ray diffraction is calculated from gas-phase H2 pumped to various electronic, vibrational, and electronic states. This is expanded upon for polyatomic molecules using the harmonic approximation for the vibrational states.

No description available.

The initial aim of the work presented in this thesis was to increase the soft x-ray quantum detection efficiency of a tandem-pair microchannel plate detector by the use of a CsI deposition photocathode. This aim was achieved. The coating technique and initial measurements are presented herein. After showing the use of such photocathodes, we investigated their stability and reproducibility. The effects of storage in poor vacuum, high vacuum and desiccated air are presented as is the stability of CsI photocathodes under prolonged X-ray bombardment. One consequence of the use of CsI is that a degree of energy resolution can be conferred upon a microchannel plate detector. We present further research in this field, including measurements performed on detectors with eight micron diameter channels. A feature of microchannel plate operation that is undesirable is the phenomenon of gain degradation. We performed a series of lifetests on a number of microchannel plate detectors.