This research was able to identify a wide range of elements present in fresh volcanic ash from a 2010 eruption in Indonesia using varied instrumental neutron activation analysis techniques. The ash was then leached into slightly acidic distilled water meant to simulate rainwater. This thesis focuses both on the methods used to identify the elements present in the ash, as well as the possible impacts of the results. The research included the use of both thermal and epithermal neutron irradiations from the University of Texas's TRIGA research reactor in conjunction with a high purity germanium detector (HPGe) with a Compton suppression system. The leachate was analyzed by an inductively coupled plasma mass spectrometer (ICP-MS), and the results were compared to the original material present in the ash. Several potentially toxic metals and metalloids leached out of the system at relatively high rates. For example, 2.7% of the original antimony present in the ash leached into the simulated rainwater, as well as 1.7% of the original nickel, and 0.71% of the original arsenic. However, the concentrations of the elements identified in the ash were mostly similar to average crustal rock, and the concentrations of the elements identified in the leachate were not determined to be at toxic levels. The total amount of each element released during the eruption was also calculated based on the estimate of 160 million tonnes of ash released during the eruption, which was determined by a different study. / text

Introduction A method based on neutron activation is being developed to assist in resolving discrepancies between the expected yield and actual yield of radionuclides produced with the vertical-beam target station (VBTS) at iThemba LABS. The VBTS is routinely employed for multi-Ci batch productions of the radionuclide pairs 22Na/68Ga and 82Sr/68Ga using standardized natMg/natGa and natRb/natGa tandem targets, respectively [1]. The metal-clad target discs are bombarded with a primary beam of 66 MeV protons at an intensity of nominally 250 µA. The encapsulation materials are either Nb (for Mg and Ga) or stainless steel (for Rb) which serve to contain the molten target materials during bombardment and act as a barrier to the high-velocity cooling water which surrounds the targets in a 4π geometry. The natRb/natGa targets are typically bombarded according to a two-week cycle while natMg/natGa targets are bombarded on an ad-hoc basis, depending on a somewhat unpredictable 22Na demand. A too-large deviation between expected yield and actual yield has at times plagued this programme. These deviations can manifest both as an apparent loss or an apparent gain (relative to the expected yield) by up to about 15% in either direction. The resulting uncertainty of up to 30% (in the worst case) from one production batch to another can be costly and is unacceptable in a large-scale production regimen. This phenomenon is believed to be brought about by two types of problems: (1) Production losses, e.g. during the radio-chemical separation process or incomplete recovery of activated target material during the decapsulation step. (2) Incorrect values obtained for the accumulated proton charge. A problem of type (1) will always result in a loss of yield. A problem of type (2) can manifest as an apparent loss or gain. In an effort to get a handle on this second type of problem, neutron activation of suitable material samples, embedded in a target holder, is being investigated as an independent indicator of the total yield. For this purpose, samples of Co, Mn, Ni and Zn were activated during production runs and Co was found to be the most appropriate. Preliminary results will be presented after first discussing why the determination of the accumulated pro-ton charge is a problem with the VBTS. Materials and Methods The VBTS consists of a central region in which a target holder is located during bombardment as well as two half-cylindrical radiation shields which completely surround the target. The shields can be moved away from the central region on dedicated rails, e.g. when repairs or maintenance is required. FIGURE 1 shows the VBTS with the shields moved to the “open” position. As some components of the station are located below the vault floor, with the target position near floor level, it proved difficult to electrically isolate the VBTS as was done for the two horizontal-beam target stations at iThemba LABS [1]. The VBTS does not act as a Faraday cup like the other target stations. Instead, the beam current and accumulated charge is measured by means of a calibrated capacitive probe [1,2]. There appears to be a variation in the response of the capacitive probe, sensitive to the beam microstructure, in particular a dependence on the beam packet length. This problem is not yet fully resolved. FIGURE 2 (a) shows the beamstop of a VBTS target holder with several Co samples mounted on the outside as well as one each of Ni, Mn and Zn. The samples are small “tablets” with a 10 mm diameter and 1 mm thickness. The reactions of interest are 59Co(n,γ)60Co, 59Co(n,3n)57Co, nat-Ni(n,X)60Co, natNi(n,X)57Co, natZn(n,X)65Zn and 55Mn(n,2n)54Mn. The relevant half-lives are 60Co(5.271 a), 57Co(271.8 d), 65Zn(244.3 d) and 54Mn(312.2 d). The half-life should be long compared to the two-week cycle in order to reduce the dependence on the exact beam history, which is very fragmented over any production period. In this respect, 60Co is considered to be particularly attractive as its long half-life of more than 5 years leads to a negligible effect by the beam history. Note that the tandem targets, shown in FIGURE 2 (b), are mounted just upstream of the beamstop – in fact, the targets and beamstop form a single unit before being fitted into the target holder. At the end of bombardment, all samples were assayed for their characteristic γ-emissions using standard off-line γ-ray spectrometry with an HPGe detector connected to a Genie 2000 MCA. Calculations of the neutron fluence density in the central sample volume on the beamstop were also performed using the Monte Carlo radiation transport code MCNPX. For these calculations, the entire VBTS, a Rb/Ga target and the vault walls were included in the model. Results and Conclusion All samples activated significantly – copious amounts of 60Co were detected in the Co discs after a two-week run. The neutron fluence density for the case of a 250 µA, 66 MeV proton beam on a natRb/natGa tandem target is shown in FIGURE 3. The dominance of low-energy neutrons is evident, which is in part due to the large amount of paraffin-wax shielding material in close proximity to the target. While reactions such as the (n,2n) and (n,3n) would be sensitive to the more energetic part of the neutron spectrum, the (n,γ) capture reaction benefits from the large low-energy component. This explains the copious amounts of 60Co formed. It was therefore decided to only retain the central Co sample for subsequent bombardments, as shown in FIGURE 4. The first results are shown in TABLE 1. The accumulated charge as obtained from the capacitive probe (Q), the specific 60Co activity (A) at the end of bombardment (EOB), and their ratio (A/Q) are presented in the table, together with the deviation of individual ratios relative to their average for the case of the Mg/Ga tandem tar-gets only. Note that all samples were counted until the statistical uncertainties were negligible. Any systematic uncertainties are ignored at this stage as they are considered to remain the same from one batch production to another. For the sake of argument, the average value of the ratio is taken as the expected value. A positive deviation of the A/Q value is then indicative of a too-small value of the accumulated charge obtained from the capacitive probe, leading to a corresponding overproduction. Likewise, a negative value is indicative of a too-large value of the accumulated charge, leading to a corresponding underproduction. It is certainly true that the data in TABLE 1 are currently very limited. It is envisaged, however, that with time the growing database of values will assist in reducing the uncertainty in determining the accumulated charge and reduce the discrepancies between predicted and actual yields significantly. TABLE 1 illuminates the underlying problem satisfactorily. The four Mg/Ga tandem target bombardments, on identical targetry, were performed successively. The neutron activation correlates well the with actual yields, pointing directly to the current integration as the main source of error. The method already proves to be useful. An indication of an over or underprediction can be obtained prior to the target processing by recovering and measuring the Co disc. This in-formation can be used to make a decision concerning the present batch production and/or the subsequent one. One can either add beam to the present production target and/or in-crease/reduce the total beam on the subsequent production target to compensate for an expected overproduction or shortfall. In conclusion, we would like to stress that the capacitive probes show great promise and that better understanding and/or possibly some development of their signal processing algorithm may improve their ability to measure the accumulated charge to the desired accuracy. Segmented capacitive probes used at iThemba LABS and elsewhere for beam position measurement [1,3] are not affected by beam microstructure as only the ratios of the signal strengths on the different sectors are important. In this case, changes in response affect all sec-tors equally and the ratios are unaffected.

Der Reaktordruckbehälter (RDB) zählt zu den nicht auswechselbaren Komponenten eines Kernkraftwerkes (KKW). Durch die hohen Neutronen- und Gammaflüsse ist er beschleunigten Alterungsprozessen unterworfen, welche die Lebensdauer eines KKW bestimmen könnten. So haben neben der chemischen Zusammensetzung des RDB-Stahls vor allem die Strahlungsparameter (Neutronen- und Gammafluenzen und deren Spektren) Auswirkungen auf die Versprödungseigenschaften des RDB. Für einen sicheren Betrieb eines KKW ist es daher sehr wichtig, die mögliche Änderung des Materialzustandes vom RDB im Voraus bewerten zu können. Die sogenannten Voreilprobenprogramme gehören deshalb zu den wichtigsten Überwachungsmaßnahmen im KKW. Mit ihnen kann die Restlebensdauer des RDB realistisch und zuverlässig beurteilt werden. In dieser Arbeit werden, neben der Bestimmung der Fluenzen an sich, auch Auswirkungen auf den Teilchenfluss in den Voreilproben, wie zum Beispiel die verschiedenen geometrischen Positionen, untersucht. Damit können mögliche Unsicherheiten bei der Bestimmung der realen Fluenzwerte abgeschätzt werden. Die Berechnungen wurden sowohl mit dem Code TRAMO als auch mit dem Code DORT durchgeführt. Die berechneten Ergebnisse wurden an Aktivierungsmonitoren, die an der RDBAußenoberfläche des KKW Kola, Unit 3 (WWER-440/213), bestrahlt wurden, überprüft. Hauptsächlich kamen Aktivierungsmonitore mit den Reaktionen 54Fe(n,p)54Mn und 58Ni(n,p)58Co zum Einsatz. Die Aktivitätsmessungen wurden vom russischen Partner, dem „Scientific and Engineering Centre for Nuclear and Radiation Safety“ (SEC NRS) durchgeführt. Es konnte gute Übereinstimmung sowohl zwischen den deterministischen und den stochastischen Berechnungsergebnissen als auch zwischen den berechneten und gemessenen Ergebnissen erzielt werden. Die durchschnittliche Differenz zwischen gemessenen und berechneten Werten betrug nur 5%. Ein Einfluss der Bestrahlungskanäle und der Versteifungsrippen der Kernumfassung auf die Monitoraktivität konnte festgestellt werden. Für die Voreilproben im Bereich des Flussmaximums wurden für den Neutronenfluss E> 0.5 MeV ein Mittelwert von rund 2.45*1012 Neutronen/cm2 berechnet. Dabei können die Unterschiede in Abhängigkeit von der Ausrichtung der Proben zum Reaktorkern bis zu 20% betragen. Abweichungen bis zu 10% können durch die Änderung der Position der Bestrahlungskapseln im Kanal entstehen. Auf Basis dieser Rechnungen wurden die Voreilfaktoren der Bestrahlungsproben bestimmt. Bei mittleren Zykluslängen würde die „End of Life“-Fluenz in den Bestrahlungsproben bereits nach 2 Jahren erreicht werden. Der berechnete maximale Gammafluss beträgt rund 3.4*1012 g/cm2s für E > 1.0 MeV und rund 8.4*1012 g/cm2s für E > 0.5 MeV, wobei der größte Anteil des Flusses (rund 97%) aus Neutronenreaktionen stammt. Damit sind die Gammaflüsse in den Proben zwei bis drei Mal so groß wie die der Neutronen. Trotzdem spielt die Materialschädigung durch die Gammastrahlung eine untergeordnete Rolle, da die DPAQuerschnitte (displacement per atom) von Gammas um etwa zwei bis drei Größenordnungen kleiner sind. Des Weiteren wurde untersucht, ob mögliche Ausheilprozesse durch zu hohe Temperaturen in den Bestrahlungsproben stattfinden könnten. Zu diesem Zweck wurde der Energieeintrag in den Bestrahlungsproben basierend auf den berechneten Teilchenflüssen bestimmt und mit einfachen thermohydraulischen Modellen die mögliche Aufheizung ermittelt. Eine Temperaturerhöhung von rund 20 K wurde mit einem konservativen Ansatz berechnet. Unter vergleichsweise realistischen Bedingungen reduzierte sich die Aufheizung auf unter 5 K. / Reactor pressure vessels (RPV) are non-restorable equipment and their lifetime may restrict the nuclear power plant-life as a whole. Surveillance specimen programs for RPV materials are among the most important measures of in-service inspection pro-grams that are necessary for realistic and reliable assessment of the RPV residual lifetime. In addition to the chemical composition of the RPV steel, the radiation pa-rameters (neutron and gamma fluences and spectra) have the most important impact on the RPV embrittlement characteristics. In this work, different geometric positions which have influence on the radiation conditions of the samples are investigated. Thus, the uncertainties can be determined in the fluence values of surveillance specimens. The fluence calculations were carried out by the codes TRAMO and DORT. This study was accompanied by ex-vessel neutron dosimetry experiments at Kola NPP, Unit 3 (VVER-440/213), which provide the basis for validation of calculated neutron fluences. The main neutron-activation monitoring reactions were 54Fe(n,p)54Mn and 58Ni(n,p)58Co. The activity measurements were carried out by “Scientific and Engineering Centre for Nuclear and Radiation Safety (SEC NRS). Good agreement between the deterministic and stochastic calculation results as well as between the calculations and the ex-vessel measurements was found. The aver-age difference between measured and calculated values is 5%. The influence of the channels for surveillance specimens and the shielding effect of a baffle rib on the monitors and on the Monte-Carlo calculated results was studied. For the surveillance specimens in the maximum of the flux, an average flux of around 2.45 * 1012 neutrons/cm2 was calculated for the neutron flux E> 0.5 MeV. The differences in the surveillance specimens could be up to 20% depending on the direction to the core. Discrepancies up to 10% can be caused by the change of the position of the capsules in the irradiation channel. Based on these calculations the lead factor of specimens was determined. The maximum fluence of RPV may be achieved after two cycles. The calculated maximum gamma flux is around 3.4 * 1012 g/cm2s for E> 1.0 MeV and around 8.4 * 1012 g/cm2s for E> 0.5 MeV, with the largest part of the flux (around 97%) from the neutron reactions. The gamma fluxes in the surveillance specimens are two to three times bigger than the neutron fluxes. Nevertheless, the material damage by the gamma radiation is very small, because the dpa (displacement per atom) cross sections of gamma rays are about two to three orders of magnitude smaller. In order to exclude the possibility of healing effects of the samples due to excessive temperatures, the heat release in the surveillance specimens was determined based on the calculated gamma fluences. The analytic treatment of the heat conduction equation and simplified SS geometries were adopted to calculate the range of tem-peratures to be expected. The temperature increase of 20 K above the inlet coolant temperature was estimated using a conservative approach. Under comparatively re-alistic conditions, the heating was reduced to less than 5 K.

This study has attempted to examine third and fourth century pottery supply in northern England together with other aspects of pottery assemblages in the region. The pottery kilns of the East Yorkshire industries have been characterised by neutron activation analysis which has proved reasonably successful in discriminating between them. Neutron activation analysis has also been utilised to attempt to check visually identified fabric groups and to help isolate other fabrics. This has been of varying success. Quantified data has been collected from 15 sites across the north and the limited published quantitative data have been utilised to examine the distribution, marketing and competition between fabric types in the region. Examination of functional variations through time between different types of site has also been undertaken as has that of variations in the quantity of finewares through time and between different types of site together with an attempt at quantifying decoration and examining trends in this. Pottery supply to the northern frontier area would seem to have been organised by different mechanisms in different periods. In the second century much of the pottery used on the frontier would appear to have been produced by the military themselves whilst in the third century and earlier fourth century free market mechanisms would seem to have operated, but in the late fourth-early fifth centuries some form of 'military contract' would appear to have taken over supply. Functional variations between different types of site have been identified with rural sites, turrets and Signal Stations sharing a major emphasis on the jar as the basic ceramic form and more complex settlement types having more diversified functional groups. The distribution of finewares also seems to be concentrated on more complex settlement types. It is apparent that there are consistent differences between the East Yorkshire region and the rest of the study area which may well reflect differences extending back into the Iron Age. Similarly there seem to be indications of some 'de-Romanisation' in late Roman assemblages but this does not develop in the fifth century, when nearly all the strands of evidence of Romano-British material culture disappear very rapidly.

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