The isotopes 238 U, 234 U and 230 Th, as members of the uranium-radium decay chain, are fractionated in the environment by changes of geochemical conditions, and they can be used for dating of recent or past geochemical processes in the Quaternary. Samples of water with uranium and of water-activated solids were taken of radioactive mineral water springs at two study sites in the area of Krkonoše-Jizera crystalline complex: Svatý Vojtěch (St. Adalbert) in Horní Malá Úpa, and Bukový Pramen in the Těsný důl valley in Janské Lázně. Uranium was co-precipitated in field conditions with hydroxides of FeIII+ in 50-liter water samples of the radioactive springs. In the lab, uranium and thorium were separated from water precipitates, as well as from solid samples after their chemical decomposition, using chromatographic extraction agent UTEVA. All the three isotopes of interest emit alpha particles, and so their activities were measured by alpha spectrometry and expressed as 234 U/238 U and 230 Th/234 U ratios. As an internal standard, 232 U/228 Th was used. The resulting 234 U/238 U activity ratios of four water samples measured ranged from 1.0747 to 1.423. In twelve samples of solid phases activity ratios 234 U/238 U from 0.861 to 1.129 were determined. The 230 Th/234 U activity ratios form two distinct...

In the analysis of environmental samples for uranium and thorium pollutants and at natural levels for the dating of geological samples there was felt a need to develop better uranium and thorium separation procedures to replace the established anion exchange method used at AEA Technology plc. This was the first aim of the PhD research. Separation of uranium from thorium prior to measurement of the isotopes by alpha spectrometry was necessary due to the similar alpha energies of234U and 230Th. TRU and UTEVA extraction chromatography resins (EIChroM Industries) were investigated as potential replacements to the anion exchange separation method. The resins are claimed by EIChroM to offer the advantage of providing an actinide specific separation while reducing the separation time from 2 to 0.5 days; the volume of acidic waste produced by a factor of 3, therefore, the cost of analysis was reduced. A uranium and thorium separation procedure using the UTEVA extraction chromatography resin was developed. The uranium and thorium were sorbed by the UTEVA resin from 2M nitric acid. The thorium was then eluted from the resin with 5M hydrochloric acid and the uranium with 0.02M hydrochloric acid. The separation procedure was then evaluated using uraninite ore, coral, granite and lake sediment reference materials. The uranium and thorium concentrations and the 234U/238U and 23oTh/234U activity ratio values determined for the reference material were in good agreement with certified values. The presence of plutonium was found to interfere with the measurement of uranium and thorium by alpha spectrometry. This was due to the similar alpha energies of uranium, thorium and plutonium. The co-elution of plutonium with uranium and thorium from the UTEVA resin was prevented by the inclusion of a reduction step using iron (Il) sulphamate. The resulting plutonium (Ill) was not retained by the UTEVA column. The chemical recoveries for the procedure were similar to those for anion-exchange, but the extraction chromatography procedure provided a more rapid separation using less reagents.

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The purpose of this project was to design, construct, and evaluate an alpha spectrometer based on an inexpensive p-i-n photodiode as a radiation detector. The BPX-61 p-i-n photodiode was selected and calculated to have a 93 µm wide sensitive volume at 25 V reverse bias. Electronics consisting of a charge-sensitive preamplifier, a pole-zero canceling CR-(RC)4 pulse shaping amplifier, and an adjustable detector bias voltage supply were devised and assembled. Several alpha spectra were recorded from different alpha radiation sources to determine the performance of the alpha spectrometer. The results show that the alpha spectrometer could successfully and accurately measure alpha spectra, which could then be used to identify radioactive materials present in the sources. An FWHM resolution of about 230 keV was measured for 5.486 MeV alpha particles from Am-241. This resolution is inferior to most alpha spectrometers that measure under vacuum. However, because the device does not require a vacuum pump and uses USB for power and data acquisition, it is a convenient and compact option for field measurements. The low cost and reasonable performance of commercial p-i-n photodiodes as radiation detectors could be appealing for future alpha spectroscopy applications.

Le projet SPIRAL2 permettra de produire au GANIL des faisceaux radioactifs et stables très intenses. Repoussant les limites actuelles de nos connaissances, il constitue une opportunité pour de nombreux domaines de la physique nucléaire. Le Super Séparateur Spectromètre S3 et son système de détection au plan focal SIRIUS ont été conçus afin de tirer le meilleur parti de ces faisceaux stables intenses notamment au profit des recherches sur les éléments N=Z proches de l'étain-100 et des noyaux super lourds. Ce travail de thèse portent sur les détecteurs silicium Tunnel de SIRIUS, avec d'un côté des simulations GEANT4 de l'ensemble de SIRIUS et d'un autre côté son pendant expérimental avec l'étude des prototypes des Tunnel de SIRIUS. Les simulations ont permis, outre la caractérisation de l'efficacité de détection et des limites induites en terme de conception mécanique, de mettre en lumière le bond en avant permis par l'avènement de détecteurs silicium presque sans zones mortes. La partie dédiée aux manipulations commence par la présentation du banc de test mis en place à l'IPHC pour recevoir et tester les détecteurs prototypes et pré-série. Le détecteur Tunnel est également présenté dans son contexte scientifique et technique. Les études des prototypes de détecteurs Tunnel et les résultats obtenus sont détaillés. Enfin, l'évolution vers les détecteurs de série est présentée sur la base des améliorations réalisées et constatées pour le détecteur de pré-série. / The SPIRAL2 project will enable the production at GANIL of very intense radioactive and stable beams. Pushing the present-day limits of knowledge, it represents an opportunity for several fields of nuclear physics. The Super Separator Spectrometer S3 associated to its focal-plane detection system SIRIUS will take the best possible benefit of these intense stable beams especially for researches on the N=Z nuclei close to Tin-100 and on the super heavy elements. This thesis is dedicated to the SIRIUS Tunnel silicon detectors, with GEANT4 simulations and their corresponding experimental study of the SIRIUS Tunnel detectors prototypes. In addition to the detection efficiency characterization and the setting of corresponding limits on mechanical conceptual drawings, the simulations have enabled to shed light on the major forward step brought by zero dead-layer silicon detectors. The section dedicated to the manipulations starts with the presentation of the test bench set up at IPHC in order and test the prototypes and pre-series detectors. The Tunnel detector is also presented in its scientific and technical context. The Tunnel detector prototypes studies and the results obtained are detailed. Finally, the evolution toward series detectors is presented on the basis of the improvements done with the pre-series detector.