Mass spectrometers are analytical instruments that convert neutral atoms and molecules into gaseous ions and separate those ions according to the ratio of their mass to charge, m/z. The measurement is reported as a mass spectrum: a plot of relative intensity vs. m/z that can be used to deduce the chemical structure and composition of materials and compounds. Initially, the use of mass spectrometers was restricted to the analysis of volatile compounds. Recent advances in the development of ionisation techniques to produce intact molecules directly from samples in the liquid or solid phase, has extended the powerful use of mass spectrometry to compounds of increasingly higher molecular mass. The aim of this study was twofold: develop diagnostic techniques for the in-situ measurement of isotope ratios in laser isotope separation experiments; and to correlate it with the measured isotope ratios on the collected product. The outcome is a thesis that can be divided into two distinct fields of application: Firstly; the Atomic Vapour Laser Isotope Separation (AVLIS) of lithium, and secondly the Molecular Laser Isotope Separation (MLIS) of uranium, In both AVLIS and MLIS pulsed laser systems were used to ionise and/or dissociate atomic or molecular beams. The pulsed nature of the lasers is ideally suited to in-situ time-of-flight detection of the produced ions. Different types of inter-changeable ion sources are common to the same TOF mass spectrometer. Each of these sources is selected according to its application. For instance, applications vary from photo- and multiphoton ionisation (laser ionisation) to surface analysis (laser desorption or particle bombardment) to chromatography (electron impact ionisation). Four different source configurations were considered in this study: (i) Atomic Laser Isotope Separation (AVLIS) of lithium; (ii) Multiphoton Ionisation (MPl) of UF6 gas; (iii) Non-resonant ionisation during Laser Desorption (LDI) of solids; and (iv) Matrix-Assisted Laser Desorption (MALD) of biopolymers. The design of each of these sources will be discussed in detail in chapters to follow. Bulk analysis of harvested laser-produced products needs to be in correlation with in-situ analysis. Three different characterisation methods were used in this study: (i) Laser Desorption Time-of-Flight Mass Spectrometry (LD-TOF-MS) (ii) Quadrupole-based Secondary Ion Mass Spectrometry (SIMS); and (iii) TOF-MS-based Secondary Ion Mass Spectrometry (TOF-SIMS). Chapter I describes the principles of time-of-flight mass spectrometry, design parameters, as well as the instrumentation that were designed and constructed for the purposes of this study. Chapter II describes the principles of Secondary Ion Mass Spectrometry (SIMS). In particular, research done on the establishment of tools to the non-expert user of SIMS to select analyses conditions, is described. Chapter III reports on the application of TOF-MS and SIMS during the AVLIS of lithium. Chapter IV reports on the application of the different combinations of TOF-MS, LD-TOF-MS, SIMS, and TOF-SIMS during the MLIS of uranium. / Thesis (Ph.D.)-University of Natal, Durban, 1999.

This thesis is based on experimental results from measurements on methyl halides at a photon energy corresponding to the He IIβ emission line. Double ionization processes involving the valence electrons of the molecules CH3F, CH3Cl and CH3I are studied by means of a magnetic bottle TOF-PEPECO spectrometer. Resulting double ionization data of these molecules suggest that mainly direct double photoionization is observed as a continuous energy sharing between the ejected electron pairs. As a mean to further understand the double ionization processes, a "rule of thumb", for double ionization in molecules, is applied to the data presented in the double ionization spectra. This is done in order to quantify the effective distance between the two vacancies created in the dications. It is found that the distance between the vacancies may be related to the bond distance between the carbon and halogen atoms. Further investigations call for quantum chemical calculations to scrutinize this hypothesis. / Det här examensarbetet är baserat på experimentella fotojonisations studier av metyl halider vid en fotonenergi motsvarande He IIβ emissionslinjen. Valenselektronerna i dubbeljonisations processerna för CH3F, CH3Cl och CH3I har studerats under användning av en så-kallad magnetisk flask TOF-PEPECO spektrometer. Resultaten av dessa mätningar visar att mestadels direkt dubbeljonisation processer före- kommer, där elektronerna delar kontinuerligt på energin som friges vid jonisationen. Den dubbla jonisa- tions processen är ytterligare studerad genom att tillämpa en tumregel för dubbeljonisation i molekyler, vilket ger en indikation av hur stort avståndet är mellan de två vakanserna som skapades när molekylerna joniserade. Resultaten från tumregeln visar att avståndet mellan vakanserna kan vara relaterade till bind- ningsavståndet mellan kol-atomen och halogen-atomen, i respektive metyl halogen. För att ytterligare bekräfta dubbeljonisations processerna i dessa molekyler, krävs kvantmekaniska beräkningar.

In zukünftigen kerntechnischen Anlagen können die Materialien Blei und Bismut eine größere Rolle spielen als heute. Für die Planung dieser Anlagen werden verlässliche Wirkungsquerschnittsdaten benötigt. Insbesondere der Neutronentransport in einem Blei-Spallationstarget eines beschleunigergetriebenen unterkritischen Reaktors hängt stark von den inelastischen Streuquerschnitten im Energiebereich von 0,5 MeV bis 6 MeV ab. In den vergangenen 20 Jahren wurden elastische und inelastische Neutronenstreuquerschnitte mit hoher Präzision für eine Vielzahl von Elementen am PTB-Flugzeitspektrometer gemessen. Zur Erzeugung der Neutronen wurde hauptsächlich die D(d,n)-Reaktion genutzt. Aufgrund des Q-Wertes der Reaktion und der verfügbaren Deuteronenenergien können Neutronen im Energiebereich von 6 MeV bis 16 MeV erzeugt werden. Die Messung von Wirkungsquerschnitten bei niedrigeren Energien erfordert somit die Verwendung einer anderen neutronenerzeugenden Reaktion. Hierfür wurde die 15N(p,n)15O-Reaktion ausgewählt, da sie die Erzeugung monoenergetischer Neutronen bis zu einer Energie von 5,7 MeV erlaubt. In dieser Arbeit wird die 15N(p,n)-Reaktion auf ihre Eignung als Quelle monoenergetischer Neutronen in Streuexperimenten untersucht. Die Untersuchung der Reaktion beinhaltet die Messung von differentiellen Wirkungsquerschnitten für ausgewählte Energien und die Auswahl von optimalen Targetbedingungen. Differentielle elastische und inelastische Neutronenstreuquerschnitte wurden unter Anwendung der Flugzeitmethode für Blei bei vier Energien zwischen 2 MeV und 4 MeV gemessen. Eine Bleiprobe mit natürlicher Isotopenzusammensetzung wurde verwendet. Für den Nachweis der gestreuten Neutronen wurden NE213 Flüssigszintillatoren verwendet, deren Nachweiswahrscheinlichkeit gut bekannt ist. Winkelintegrierte Wirkungsquerschnitte wurden mit einem Legendre-Polynomfit unter Verwendung der Methode der kleinsten Quadrate bestimmt. Zusätzlich erfolgten Messungen für die isotopenreinen Streuproben 209Bi und 181Ta bei 4 MeV Neutronenenergie. Die Ergebnisse werden mit denen früherer Experimente und aktuellen Evaluationen verglichen. / In future nuclear facilities, the materials lead and bismuth can play a more important role than in today’s nuclear reactors. Reliable cross section data are required for the design of those facilities. In particular the neutron transport in the lead spallation target of an Accelerator-Driven Subcritical Reactor strongly depends on the inelastic neutron scattering cross sections in the energy region from 0.5MeV to 6 MeV. In the recent 20 years, elastic and inelastic neutron scattering cross sections were measured with high precision for a variety of elements at the PTB time-of-flight spectrometer. The D(d,n) reaction was primarily used for the production of neutrons. Because of the Q value of the reaction and the available deuteron energies, neutrons in the energy range from 6MeV to 16MeV can be produced. For the cross section measurement at lower energies, however, another neutron producing reaction is required. The 15N(p,n)15O reaction was chosen, as it allows the production of monoenergetic neutrons with up to 5.7MeV energy. In this work, the 15N(p,n) reaction was studied with focus on the suitability as a source for monoenergetic neutrons in scattering experiments. This includes the measurement of differential cross sections for the neutron producing reaction and the choice of optimum target conditions. Differential elastic and inelastic neutron scattering cross sections were measured for lead at four energies in the region from 2MeV to 4MeV incident neutron energy using the time-offlight technique. A lead sample with natural isotopic composition was used. NE213 liquid scintillation detectors with well-known detection efficiencies were used for the detection of the scattered neutrons. Angle-integrated cross sections were determined by a Legendre polynomial expansion using least-squares methods. Additionally, measurements were carried out for isotopically pure 209Bi and 181Ta samples at 4MeV incident neutron energy. Results are compared with other measurements and recent evaluations.

Thesis (Ph. D.)--University of Washington, 2007. / Vita. Includes bibliographical references (p. 161-186).

Thesis (M. S.)--Chemistry and Biochemistry, Georgia Institute of Technology, 2006. / Fernandez, Facundo, Committee Chair ; Janata, Jiri, Committee Member ; Mizaikoff, Boris, Committee Member.

Includes bibliographical references (p. 162-177).

The fragmentation of a 133 pps beam of 14Be ions at 35 MeV/A on targets of carbon and lead has been used to study the structure of the unbound nucleus 13Be. Neutrons and 12Be reaction products were measured in the DeMoN array and a detector telescope placed at 0° respectively. These coincidence measurements were used to reconstruct the 13Be particles. The beam energy was measured on a particle by particle basis from the time of flight. This was essential for momentum measurements which were made in the reference frame of the projectile. A significant contribution to the experimental background came from reactions in the detector telescope, which had to be subtracted. Relative velocity (arithmetic velocity difference) and invariant mass analyses both signify the existance of significant strength close to the 12Be + n threshold. Simulations including an experimental filter clearly show that this includes strength that is localised below 500 ke V in relative energy. Momentum distributions for 12Be, 10Be, neutrons and the reconstructed 13Be particle in the longitudinal direction have been measured. The 13Be distribution displays evidence for a two component structure. Calculations of the neutron stripping from 14Be have shown that this structure requires s-wave stripping to explain the narrow component. The wider component is consistent with d- wave stripping, and additional contributions from p-wave stripping cannot be excluded. The angular distribution of neutrons from 12Be + n breakup, measured in the 13Be reference frame is essentially isotropic. There is evidence for a weak asymmetry which could be due to broad over-lapping states of both positive and negative parity at energies below 2 MeV. This would support the inclusion of a P½ resonance in the low-lying structure of 13Be.

The work focuses on Monte Carlo simulations for finding the optimal back scatter time-of-flight spectrometer design for concept testing at the NESSA facility at Uppsala University. The spectrometer consists of two scintillator detectors, D1 (placed in a neutron beam) and D2 (placed in front of D1), at some distance from each other. A fraction of the neutrons that impinge on D1 back scatter into D2 and information on the neutron energy distribution is acquired using the time-of-flight method. For the given constraints on geometry, resolution and efficiency a best resolution was found to be 6.6% with a corresponding efficiency of 1E-4 which gives a sufficient count rate for a neutron generator producing 1E+11 neutrons/s. In order to achieve a minimum of 10 000 counts/h with the same setup a D2 with an area of at least 7 cm^2 is required.

Abstract The thesis clearly demonstrates that photon migration measurements allow characterization of pulp and paper properties, especially the fines and filler content of pulp, and the basis weight, thickness and porosity of paper. Pulp and paper are materials with a worldwide significance. Their properties strongly depend on the manufacturing process used. For efficient process control, the employed monitoring and measuring has to be fast. Therefore it is worthwhile to try to develop new approaches and techniques for such measurements. Recent advancements in optics offer new possibilities for such development. If two samples have different optical properties their photon migration distributions are different. The measurement of a photon migration distribution allows some features between two optically slightly dissimilar samples to be distinguished. Some simple measurements, which only yielded the photons' average time of flight, were made with an oscilloscope and a time-of-flight lidar. More precise measurements yielding photon pathway distribution or some selected characteristics like light pulse rise time, broadening, or fall time were measured with a streak camera. Two methods to assess photon path length distribution were introduced: particle determination with simulation, and streak camera with deconvolution. The basic properties for pulp are consistency and fines content and for paper the basic properties are thickness, basis weight and porosity. The influence on photon migration caused by changes in these basic properties was determined. As pulp and paper are rarely very basic, an additional property was demonstrated for both materials. For pulp it was the content of filler talc, and for paper it was the use of beaten pulp as a raw material. These additional properties were also distinguishable.

Abstract The development of a non-invasive glucose monitoring technique is very important because it would tremendously diminish the need to puncture the skin when taking blood samples and help diabetic patients in controlling their blood glucose levels and in treating Diabetes Mellitus. The focus of this thesis is on measuring the effect of glucose on the light scattering properties of a tissue-simulating phantom and biological tissues in vitro. Optical coherence tomography (OCT), the pulsed photoacoustic (PA) technique, and the time-of-flight (TOF) technique are used in the measurements and their capabilities for detecting changes in the scattering properties are evaluated and compared with each other. The theoretical background of the techniques, light propagation and PA wave generation are briefly explained. The glucose-induced changes in light scattering are also reviewed. The measurement results with the OCT and the PA technique from Intralipid, pig whole blood, and mouse skin tissue samples show that the glucose-induced changes are larger in the biological tissues than in the Intralipid phantom. The PA measurements show that although the PA signals are stronger at a wavelength of 532 nm than at 1064 nm, the glucose-induced change in the peak-to-peak value of the PA signal measured from pig whole blood is larger at a wavelength of 1064 nm than at 532 nm. The TOF measurements with a streak camera show that the scattering-related changes in the registered pulse shapes occur mainly in the rising part of the pulses. The utilization of fiber-optic measurement heads enabled the detection of back-scattered photons at different distances from the emitting fiber. Although all the techniques are able to detect changes induced by large glucose concentrations (0–5000 mg/dl) in Intralipid, the effect of glucose on the scattering properties of Intralipid is so weak that the techniques failed to detect changes with lower (50–500 mg/dl) concentrations. The measurements of biological samples with the PA technique and with the OCT also demonstrate capabilities to measure glucose concentrations in the physiologically relevant range (18–450 mg/dl) as well. The results compare well with earlier literature and also confirm some earlier findings.