Positron emission tomography (PET) employs short half-life positron emitting isotopes, typically ¹⁸F, for in vivo measurement of physiological processes. Easy access to structurally diverse radiolabelled probes would accelerate the rapid progress of PET imaging but, to date, radiochemistry is still limited by cost and efficiency. Nucleophilic fluorination with ¹⁸F-fluoride is the preferred “non-carrier-added” methodology in the synthesis of ¹⁸F-labelled pharmaceuticals because it leads to radiotracers with a high specific activity, a key feature allowing for investigations to be performed in sub-toxic doses. Chapter 1 serves as an introduction on radiochemistry, especially focussing on current radiosynthetic methods for the synthesis of ¹⁸F-labelled aromatics. Aromatic compounds without electron-withdrawing groups are notoriously difficult to label with ¹⁸F-fluoride. In this thesis, we present two novel methodologies to deliver ¹⁸F-labelled aromatic compounds from nucleophilic 18F-fluoride. Chapter 2 details the experimental efforts towards “Convergent Radiosynthesis” (Scheme 1). We proposed a convergent synthetic tactic that allows for simultaneous reaction between three or more substrates, including an ¹⁸F-labelled building block. This chemistry has been validated by the radiosynthesis of various structural scaffolds which are not responsive to direct nucleophilic fluorination. Chapter 3 presents our research into “Oxidative Nucleophilic ¹⁸F-Fluorination” (Scheme 2). We proposed that electron-rich aromatics, such as phenols, which are not responsive to nucleophilic fluorination may undergo umpolung reactivity under oxidative conditions. This “umpolung strategy” allows for the direct transformation from ¹⁸F-fluoride to 4-[¹⁸F]fluorophenol. Potentially, this established oxidative fluorination strategy could be adapted to the radiosynthesis of radiotracers containing a 4-fluorophenol sub-motif, such as 6-fluoro-meta-tyrosine. An appropriate precursor has been validated for the prospective radiosynthesis of 6-[18F]fluoro-meta-tyrosine.

Thesis (M. Phil.)--University of Hong Kong, 2007. / Also available online.

Thesis (M. Phil.)--University of Hong Kong, 2007. / Title proper from title frame. Also available in printed format.

Thesis (M. Phil.)--University of Hong Kong, 2007. / Title proper from title frame. Also available in printed format.

Thesis (Ph. D.)--University of Hong Kong, 2006. / Title proper from title frame. Also available in printed format.

Thesis (Ph. D.)--University of Hong Kong, 2010. / Includes bibliographical references (leaves 121-127). Also available in print.

Thesis (M. Phil.)--University of Hong Kong, 2002. / Includes bibliographical references (leaves 111-112).

Secondary electron (SE) emission from thin carbon foils induced by 1-20 keV positrons has been investigated over a range of nominal foil thicknesses from 1.0 to 5.0 μg/cm2. The measurement of SEs was carried out in forward geometry using a microchannel plate as a detector. The SE yield γ has been measured as a function of beam energy and compared with some Monte Carlo simulation results. We also present in this thesis the material parameter Λ=? / (dE / dx) and the emitted SE energy spectra. Forincident positron energy of 5 keV or higher, the distribution is found to be characterizedby the Sickafus form, AEm and m is close to 1. For low energy incident positrons however, another form, Bexp(E / t) , is proposed for describing the SE distribution. The maximum scattering angle for SEs emitted from 5.0 μg/cm2 is found to be around 60°. Measurements of energy loss and energy loss straggling for 1-10 keV positrons passing through thin carbon foils of different thicknesses ranging from 1.0 to 5.0 μg/cm2 are present in this thesis. The stopping power dE / dx and positron transmission coefficient have also been investigated as a function of incident positron energy and foil thickness. Particularly, our experimental results are compared with those from Monte Carlo simulation and theory with a view to providing a way to determine the real thickness of carbon foil. The ratio of the energy loss straggling to the foil thickness seems to have a linear relation with the beam energy. The transmitted positrons after passing through 5.0 μg/cm2 C-foil have a small scattering angle which is less than 10°. Titanium dioxide nanotube arrays fabricated by anodization of titanium foil and annealed at different temperatures were studied using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and positron annihilation spectroscopy (PAS). The crystallization process and morphological change of the nanotubes have been discussed. It is found that anatase (101) only appeared on the walls of the nanotube. The atomic concentration of fluoride and the ratio of Ti/O decreased when the annealing temperature increased. Vacancy type defects were found to diffuse toward the surface when the samples were annealed at 200°C and 400°C and healing of vacancies occurred at 600°C. In addition, the fluoride may form some complexes with vacancies on the surface hence lowering the value of the S parameter. A new design of the lifetime positron beam based on the SE emission is proposed. The observed experimental results and simulation results make it possible to construct a new type of high resolution (<250ps) lifetime positron beam. In addition, how rastering of the positron beam can be used to accurately locate the position of the C-foil is also shown; a feature that will be of value in setting up a positron lifetime system. Such a lifetime system is expected to be much simpler in construction than existing beam based lifetime spectroscopy systems. / published_or_final_version / Physics / Doctoral / Doctor of Philosophy

A proposed design of the variable energy positron annihilation spectroscopy (VEPALS) system based on secondary electron (SE) emission from a thin carbon foil has been investigated practically. The SE yield and the positron transmission coefficient were investigated as a function of the positron beam energy, the annular electrode potentials, and the column lengths of the annular electrode. The positron lifetime spectra of single crystal p-type silicon(Si) sample under different annular electrode potentials were analyzed. The result gives a supposed annular electrode potential of 1.5 kV. In view of this, the positron lifetime spectra were measured under different positron beam energy by fixing the annular electrode potential. It can be seen that all the spectra have the main p-type Si bulk lifetime component of 234 ps occupying more than 60% intensities. The intensity of the 234 ps component reaches up to 84.5 ±1.3 % when the positron beam energy is 15 keV. Further, the origin of the satellite peaks in the positron lifetime spectra are also investigated. It has been shown that the satellite peaks is attributed to the overflowing positrons on the MCP detector. The single crystal strontium titanate (STO) substrates after vacuum annealing treatment have been investigated in detail by several experimental techniques. The crystallization changes induced by the vacuum annealing were investigated by X-ray diffraction(XRD). Secondary phases were occurred after annealing treatment. The measured X-ray photoelectron spectroscopy (XPS) at O1s and C1s core levels were analyzed. The additional peaks after annealing are attributed to hydroxyl species, C-OH compounds, and carbonates. The variable energy Doppler broadening spectroscopy (VEDBS) and the traditional coincidence positron annihilation lifetime spectroscopy (PALS) were used to probe defects in STO samples. For long annealing time samples, the S parameters decrease below the reference level. The S-Wplot suggests that almost the same type of vacancy defects were induced during the annealing treatment. The positron lifetime results suggest that the main defects in annealed samples are oxygen monovacancies or divacancies and Sr-O vacancy complexes. The sample with annealing time of 110h has minimum positron effective diffusion length and maximum average lifetime, which is attributed to the increase of the vacancy-type defects during the long annealing treatment. / published_or_final_version / Physics / Master / Master of Philosophy

published_or_final_version / abstract / toc / Physics / Master / Master of Philosophy