A possible mechanism to explain the origin of around 35 neutron–deficient stable isotopes with mass A≥75 between 74 Se and 196 Hg, known as the p–nuclei is the nucleosynthesis in the proton–rich neutrino–driven winds of core–collapse supernovae via the νp–process. However this production scenario is very sensitive to the underlying supernova dynamics and the nuclear physics input. As far as nuclear uncertainties are concerned, the breakout reaction from the pp-chains, 7Be(α, γ)11C, has been identified as an important link which can influence the nuclear flow and therefore the efficiency of the νp–process. However its reaction rate is not well known over the relevant energy range (T9 = 1.5–3). In this thesis we report on the direct first measurement of two resonances of the 7Be(α, γ)11 C reaction with previously unknown strengths using an intense radioactive 7Be beam from ISAC and the DRAGON recoil separator in inverse kinematics. Since resonance strength measurements with low mass beams using recoil separators depend strongly on the recoil angular distribution, which can exceed the acceptance of the separator, we first performed a proof–of–principle test by measuring a known resonance of the 6Li(α, γ)10B reaction, which also presents a similar challenge. Our results from the 6Li(α, γ)10B reaction are in agreement with literature, showing that DRAGON can measure resonance strengths of reactions for which the maximum momentum cone of the recoils exceeds its acceptance. From the newly measured 7Be(α, γ)11C resonance strengths we calculated the new reaction rate which is lower than the current recommended by 10–50% and constrained to 5–10% in the relevant temperature region. Using this new rate, we performed detailed nucleosynthesis calculations which suggest that there is no effect the production of light p–nuclei, but a production increase for CNO elements of up to an order of magnitude is observed. / Dissertation / Doctor of Philosophy (PhD)

Dans les milieux astrophysiques explosifs tels que les novae ou les sursauts X, la densité d'hydrogène et la température sont suffisamment grandes pour que le temps entre deux réactions impliquant un proton soit plus court que le temps de vie de certains ions radioactifs. La connaissance de la section efficace des réactions de capture d’un proton par un ion radioactif est un des ingrédients important permettant la modélisation de tels milieux. Dans ce travail, un nouveau dispositif expérimental permettant d'étudier la force de résonance de réactions (p,gamma) en cinématique inverse est présenté. Ce dispositif, baptisé ARES (Astrophysical REcoil Separator), a été d’abord caractérisé à l'aide de l'étude de la réaction 19F(p,gamma)20Ne et plus particulièrement de la mesure de la force de la résonance bien connue à 635 keV au dessus du seuil 19F+p. De plus, la simulation de cette expérience est en accord avec les mesures effectuées. Une première mesure de force de résonance d'une réaction impliquant un faisceau d'ions radioactifs est ensuite présentée. Il s'agit de la réaction 19Ne(p,gamma)20Na et plus particulièrement de la résonance à 448 keV au dessus du seuil 19Ne+p. Une limite supérieure de 15.2 meV avec un niveau de confiance de 90% est obtenue. Cette limite supérieure améliore légèrement les résultats de mesures antérieures. / In explosive astrophysical environments such as novae or X-ray bursts, the temperature and the hydrogen density are so large that the time between two reactions involving protons is smaller than the live time of radioactive ions. The cross section of such reactions is an important ingredient of the modeling of such environments. In this work, a new experimental device, allowing the study of resonance strength of (p,gamma) reactions, is presented. This setup, called ARES (Astrophysical REcoil Separator), is first characterized using the study of the well known reaction, 19F(p,gamma)20Ne and more precisely the measurement of the resonance strength of the 635 keV level above the 19F+p threshold. The simulation of this experiment is found in good agreement with the measurement. Then the first resonance strength measurement of a reaction involving radioactive ions beams is presented, i.e. the resonance strength of the 448 keV level above the 19Ne+p threshold in the 19Ne(p,gamma)20Na reaction. An upper limit of 15.2 meV with a confidence level of 90% is obtained. This upper limit improves slightly the results of previous measurements.

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Secondary Ion Mass Spectrometry (SIMS) is a powerful technique for high spatial resolution chemical mapping and characterization of native surfaces. The use of massive cluster projectiles has been shown to extend the applicable mass range of SIMS and improve secondary ion yields 100 fold or beyond. These large projectiles however, present a challenge in terms of focusing due to the initial spatial and kinetic energy spreads inherent to their generation. In the present work, we describe the development and construction of a novel primary ion (PI) column employing a gold nanoparticle – liquid metal ion source (AuNP-LMIS) and the coupling to ultrahigh resolution mass spectrometers (e.g., Fourier Transform Ion Cyclotron Resonance Mass Spectrometer, FT-ICR MS) for accurate chemical characterization of complex biological surfaces. This work describes the ion dynamics, development and the experimental characterization of the AuNP-LMIS.

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Philosophiae Doctor - PhD / The Subatomic Physics Department of iThemba Laboratory for Accelerated Based Sciences (iThemba LABS) conducts experiments that require a variety of particle beams in order to study nuclear properties (reaction, structure, etc.) of various nuclides. These particle beams are accelerated using the K-200 Separated Sector Cyclotron (SSC) and delivered to different physics experimental vaults. Prior to acceleration, the particle beam is first ionised using an Electron Resonance Ion Source (ECRIS). The main goal of this study is the production of exotic metallic beams of 60Ni8+ and 62Ni8+ using ECRIS4, which are required for the Coulomb excitation experiments approved by the Programme Advisory Committee (PAC) at iThemba LABS. In order to provide the metallic beams of nickel, a development study of organometallic materials containing 60Ni and 62Ni isotopes in a form of metallocene complexes was undertaken. The nickelocene (NiCp2) complex, a member of the organometallic family, was synthesised at the Physics Target Laboratory of iThemba LABS for the first time. Method development involved the use of natural nickel during the multi-step synthesis before the use of enriched nickel-60 (60Ni) and nickel-62 (62Ni). Nine samples of NiCp2 were synthesised; two were isotopically enriched nickelocene (60NiCp2 and 62NiCp2). The percentage yields of the synthesised nickelocene samples ranged between 16 to 50 %, and samples were characterised by investigating their crystal structure and bonding arrangements in the complexes by X-ray diffraction (XRD) , Fourier Transform Infrared (FT-IR) spectroscopy, and Proton Nuclear Magnetic Resonance (1H NMR). The synthesised nickelocene were further used with ECRIS4 for the production of Ni beams on the Q-line of the cyclotron. The Metal Ions from Volatile Compounds (MIVOC) technique was used for the conversion of 60Ni and 62Ni to ion species. The method used the organometallic compounds which are volatile at specific pressures at ambient temperatures. Metallic ion beams of nickel were successfully produced after a carefully pre-sample conditioning in the MIVOC container before connecting the MIVOC set-up to the new injection system of the ECRIS4. Measured beam intensities during the experiment for both 60Ni+ and 62Ni+ were approximately 30 μA, optimum for physics measurements. The development of the MIVOC technique opens up new beam-target combinations with the use of new exotic stable beams for new science cases at iThemba LABS. Reactions in inverse kinematics, multi-step Coulomb-excitation and other types of reactions will immensely benefit from these developments.

Im Mittelpunkt der vorliegenden Arbeit stehen sehr elementaren chemische Reaktionen in der Gasphase: Elektron-Transfer Prozesse oder die Uebertragung eines einzelnen Protons. Der Schwerpunkt liegt dabei auf der Untersuchung der Reaktions-Dynamik, die sich in der Energie- und Winkelverteilung der Produkte aeussert. Neben einer schon vorhandenen Guided-Ion-Beam Apparatur, in der ein durch elektrische Hochfrequenzfelder gefuehrter Ionenstrahl mit dem Neutralgas in einer Streukammer wechselwirkt, wurde fuer die Untersuchungen eine neu aufgebaute Apparatur TITAP (Transverse Ion Trap APparatus) verwendet, in der unter Verwendung eines 22Pol Ionen-Speichers ein Streuexperiment zwischen einem Molekularstrahl von Neutralteilchen und einem stationaeren Ionentarget realisiert wird. Die Aussagen der Experimente in beiden Apparaturen ergaenzen sich dabei. Als Beispiel fuer einen Protonen bzw. Deuteronenaustausch wurden fuer die sehr fundamentale Reaktion H- + D2 -> D- + HD und ihre isotopische Variante D- + H2 -> H- + HD integrale und differentielle Querschnitte bestimmt. In guter Uebereinstimmung mit Ergebnissen einer Kreuzstrahlapparatur zeigt die Reaktion eine ausgepraegte Vorwaertsstreuung bei kleinen Stossenergien. Fuer den Elektron-Transfer konnten sowohl in einfachen dreiatomigen Systemen (Ar+ + N2, Ar+ + D2) wie auch in Reaktionen von Edelgas-Ionen mit Kohlenwasserstoffen (Ethan, Propan) Translationsexoergizitaeten bei kleinen Stossenergien (<= 1eV) bestimmt werden. Im Fall der Kohlenwasserstoffe zeigt sich bei Variation der Stossenergie im Bereich 100meV bis 5 eV nur eine geringe Aenderung der Verzweigungsverhaeltnisse fuer die entstehenden unterschiedlichen Fragmente. Die Empfindlichkeit der Speichertechnik fuer sehr langsam ablaufende Prozesse wurde am Beispiel der Feinstruktur-Relaxation von Argon-Ionen in Stoessen mit Helium bei tiefen Temperaturen gezeigt. Die neue Apparatur hat aber noch grosse Vorzuege fuer weitere geplante Projekte, wie die Untersuchung von Reaktionen mit Radikalen (Wasserstoff-, Stickstoff-, Kohlenstoffatomen) oder Elektron-Ion Rekombination.