A quantificação da atividade de radionuclídeos emissores de raios gama em amostras medidas por espectrometria gama com detectores HPGe depende da análise dos fotopicos presentes no espectro, especialmente da determinação exata das suas áreas líquidas. Tal análise é geralmente realizada com o auxílio de ferramentas de software proprietário. Este trabalho apresenta uma metodologia, descrição de algoritmos e um aplicativo de código aberto, denominado OpenGamma, para a busca e análise de fotopicos a fim de se obter seus parâmetros relevantes e as atividades dos radionuclídeos na amostra. A implementação computacional é distribuída sob licença aberta para o código principal e com o uso de pacotes de software aberto para o projeto da interface e para bibliotecas matemáticas. O procedimento para a busca de picos é realizado em três etapas. Primeiramente, executa-se uma pesquisa preliminar com o método da segunda diferença, que consiste na geração de um espectro derivado para a busca de picos candidatos. Na segunda etapa, calculam-se as larguras experimentais dos picos, dos quais escolhem-se aqueles bem formados e isolados para a obtenção da função de ajuste da largura vs. canal, por meio do método de Levenberg-Marquardt para ajustes não-lineares. Por fim, regiões do espectro com picos agrupados são delimitadas e novo ajuste não-linear é aplicado a cada região para a obtenção dos termos da linha de base e dos fotopicos. A partir destes termos, são calculadas as áreas líquidas dos picos. Para a determinação da atividade, curvas de calibração de eficiência previamente obtidas, bem como dados de transições gama dos radionuclídeos, são incorporadas ao código e aplicadas. O código foi escrito em linguagem C++ e a interface foi desenvolvida com a ferramenta Qt. Para as funções matemáticas e procedimentos de ajuste, foi usada a biblioteca científica GNU (GSL). A validação de código foi feita por meio da análise de: 1) espectros sintéticos de teste da AIEA, especialmente desenhados para a avaliação de desempenho de software; 2) espectros obtidos com amostras de exercícios de intercomparação e 3) espectros da rotina de trabalho do Laboratório de Radiometria Ambiental (LRA) do IPEN e analisados com o aplicativo comercial InterWinner. Os resultados obtidos são consistentes com os valores de referência e com aqueles obtidos pelo aplicativo citado, sugerindo que o código OpenGamma pode ser utilizado com segurança na espectrometria de raios gama de uso geral. / Radioactivity quantification of gamma-ray emitter radionuclides in samples measured by HPGe gamma-ray spectrometry relies on the analysis of the photopeaks present in the spectra, especially on the accurate determination of their net areas. Such a task is usually performed with the aid of proprietary software tools. This work presents a methodology, algorithm descriptions and an open source application, called OpenGamma, for the peak search and analysis in order to obtain the relevant peaks parameters and radionuclides activities. The computational implementation is released entirely in open-source license for the main code and with the use of open software packages for interface design and mathematical libraries. The procedure for the peak search is performed on a three step approach. Firstly a preliminary search is done by using the second-difference method, consisting in the generation of a derived spectrum in order to find candidate peaks. In the second step, the experimental peaks widths are assessed and well formed and isolated ones are chosen to obtain a FWHM vs. channel relationship, by application of the Levenberg-Marquardt minimization method for non-linear fitting. Lastly, regions of the spectrum with grouped peaks are marked and a non-linear fit is again applied to each region to obtain baseline and photopeaks terms; from these terms, peaks net areas are then assessed. For the activity determination, previously obtained efficiency calibration curves, as well as nuclides gamma-ray data, are incorporated in the code and applied. The code was developed in C++ language and the interface was developed with Qt GUI software toolkit. GNU scientific library, GSL, was employed to perform fitting procedures as needed. Validation of code was done by analyzing: 1) synthetic test spectra from IAEA, especially designed for software performance evaluation; 2) spectra obtained from samples of intercomparison exercises and 3) spectra from routine activities of the Environmental Radiometric Laboratory (LRA) at IPEN and analyzed with the commercial software package InterWinner. Results obtained are consistent with the reference values and with those obtained by the aforementioned package. The results suggest that the OpenGamma code could be safely used in general-purpose gamma-ray spectrometry.

<p><font face="TimesNewRomanPSMT"> <p align="left">Natural radioactivity studies have been carried out to study the textural characteristics, heavy mineral composition, provenance, sediment transport, and depositional environment of beach placer deposits. The naturally occurring radionuclides such as properties of beach sands, which reflect the geological characteristics such as transport and sorting processes and the depositional environment. The present work focuses on the radiometric characteristics of beach sand deposits along the west coastof South Africa. Beach sands samples were collected at the Melkbosstrand (MBS) and Ouskip (OSK) beach. The activity concentrations of these radionuclides were determined by high-resolution gamma-ray spectrometry using a high-purity germanium (HPGe) detector in a low-background configuration.</p> </font></p>

Gamma-ray spectrometry measurements performed on site, or “in situ”, is a widely used and powerful method that can be employed both to identify and quantify ground deposited radionuclides. The purpose of this thesis is to improve the calibration of high purity germanium (HPGe) detectors for in situ measurements, and calculate the combined uncertainty and potential systematic effects. An improved semi-empirical calibration method is presented, based on a novel expression for the intrinsic detector efficiency that includes both the energy and angular response of the detector. A three-layer model for the description of the depth distribution of the radionuclide and the soil density is proposed. The combined uncertainty of intrinsic detector efficiency calibrations and in situ measurements according to the proposed method was estimated. The uncertainty in the intrinsic detector efficiency was found to be 5.1 and 8.1% (coverage factor k=1, i.e. for a confidence interval of about 68%), for the two detectors calibrated. These numbers were, however, at a later stage reduced to 3.7 and 4.2%, using a revised expression for the intrinsic detector efficiency. For in situ measurements, the combined standard uncertainty was found to be 15-20% (k=1), based on the original expression for the intrinsic detector efficiency. Monte Carlo models of the two detectors were created and Monte Carlo calculated values for intrinsic detector efficiency were compared with experimental data. As a discrepancy was found, a thorough investigation of the detector response was performed. Scanning of the detector surface with a collimated 59.5 keV photon beam revealed the detector response to be highly irregular over the detector surface. It was concluded that the efficiency deficit of the detector could most likely be attributed to an increase in dead layer thickness compared with manufacturer supplied data. The thickness of the dead layer was estimated to be 1.5-1.9 mm, whereas the nominal value was 0.7 mm. Radiographs of the detectors were produced that provided valuable information about the physical dimensions of the germanium crystal, as well as its actual location within the detector housing. The Monte Carlo models were employed to calculate in situ measurement efficiencies for measurements of 137Cs deposition from the Chernobyl fallout. Results from the Monte Carlo simulations were compared both with the semi-empirical method and with soil sample data, and satisfactory agreement was confirmed. It was then proceeded to employ the Monte Carlo model to calculate the effect on in situ measurement results by two influencing parameters: ground curvature and activity in trees. Neither of these parameters was found to influence the result by more than about 25%. This deviation is comparable with the measurement uncertainty, and should not deter from measurements in such terrain.

<p><font face="TimesNewRomanPSMT"> <p align="left">Natural radioactivity studies have been carried out to study the textural characteristics, heavy mineral composition, provenance, sediment transport, and depositional environment of beach placer deposits. The naturally occurring radionuclides such as properties of beach sands, which reflect the geological characteristics such as transport and sorting processes and the depositional environment. The present work focuses on the radiometric characteristics of beach sand deposits along the west coastof South Africa. Beach sands samples were collected at the Melkbosstrand (MBS) and Ouskip (OSK) beach. The activity concentrations of these radionuclides were determined by high-resolution gamma-ray spectrometry using a high-purity germanium (HPGe) detector in a low-background configuration.</p> </font></p>

Environmental gamma-ray spectroscopy provides a powerful tool that can be used in environmental monitoring given that it offers a compromise between measurement time and accuracy allowing for large areas to be surveyed quickly and relatively inexpensively. Depending on monitoring objectives, spectral information can then be analysed in real-time or post survey to characterise contamination and identify potential anomalies. Smaller volume detectors are of particular worth to environmental surveys as they can be operated in the most demanding environments. However, difficulties are encountered in the selection of an appropriate detector that is robust enough for environmental surveying yet still provides a high quality signal. Furthermore, shortcomings remain with methods employed for robust spectral processing since a number of complexities need to be overcome including: the non-linearity in detector response with source burial depth, large counting uncertainties, accounting for the heterogeneity in the natural background and unreliable methods for detector calibration. This thesis aimed to investigate the application of machine learning algorithms to environmental gamma-ray spectroscopy data to identify changes in spectral shape within large Monte Carlo calibration libraries to estimate source characteristics for unseen field results. Additionally, a 71 × 71 mm lanthanum bromide detector was tested alongside a conventional 71 × 71 mm sodium iodide to assess whether its higher energy efficiency and resolution could make it more reliable in handheld surveys. The research presented in this thesis demonstrates that machine learning algorithms could be successfully applied to noisy spectra to produce valuable source estimates. Of note, were the novel characterisation estimates made on borehole and handheld detector measurements taken from land historically contaminated with 226Ra. Through a novel combination of noise suppression and neural networks the burial depth, activity and source extent of contamination was estimated and mapped. Furthermore, it was demonstrated that Machine Learning techniques could be operated in real-time to identify hazardous 226Ra containing hot particles with much greater confidence than current deterministic approaches such as the gross counting algorithm. It was concluded that remediation of 226Ra contaminated legacy sites could be greatly improved using the methods described in this thesis. Finally, Neural Networks were also applied to estimate the activity distribution of 137Cs, derived from the nuclear industry, in an estuarine environment. Findings demonstrated the method to be theoretically sound, but practically inconclusive, given that much of the contamination at the site was buried beyond the detection limits of the method. It was generally concluded that the noise posed by intrinsic counts in the 71 × 71 mm lanthanum bromide was too substantial to make any significant improvements over a comparable sodium iodide in contamination characterisation using 1 second counts.

Magister Scientiae - MSc / Natural radioactivity studies have been carried out to study the textural characteristics, heavy mineral composition, provenance, sediment transport, and depositional environment of beach placer deposits. The naturally occurring radionuclides such as 232Th, 238U and 40K are used as the tracers of the mineralogical properties of beach sands, which reflect the geological characteristics such as transport and sorting processes and the depositional environment. The present work focuses on the radiometric characteristics of beach sand deposits along the west coast of South Africa. Beach sands samples were collected at the Melkbosstrand (MBS) and Ouskip (OSK) beach. The activity concentrations of these radionuclides were determined by high-resolution gamma-ray spectrometry using a high-purity germanium (HPGe) detector in a low-background configuration.

This thesis deals with the idea of using accelerator driven systems for thorium transmutation into the fissile material, which can be utilized in the accelerator driven systems and in thermal nuclear reactors. Thorium occurs on Earth only in fertile isotope Th-232. It can be converted to fissile U-233 by neutron capture and subsequent beta decay. The experimental part handles the data measured by the irradiation of four thorium samples by the secondary neutrons in the QUINTA spallation target, which was irradiated with 660~MeV protons. Reaction rates for the fission and spallation products were estimated using gamma spectroscopy and activation techniques. Furthermore, Pa-233 production rates were also determined in all experimental samples. Pa-233 and fission production rates were calculated in all experimental samples using the MCNPX transport code and evaluated nuclear data for high-energy reactions. The experimental results are of a great importance for the future investigation of thorium in the accelerator driven system concept, validation of Monte-Carlo based calculation codes and validation of high-energy nuclear models.

The Master Thesis deals with the use of thorium nuclear fuel in accelerator driven systems. Basic principle of ADS, present situation and future possibilities are described in this work. The main goal of the work is determination of neutron flux in spallation target QUINTA. In December 2013, an experiment was performed at Joint Institute for Nuclear Research, Dubna. Samples of cobalt, situated at different positions in QUINTA target, were irradiated in secondary neutron field generated by deuteron beam of energies 2 AGeV and 4 AGeV and beam of C-12 with energy 2 AGeV. The samples were measured with the use of germanium semiconductor detectors and analysed using gamma-ray spectrometry. Reaction rates of Co-59 products were determined. Neutron flux was determined in setup QUINTA on the base of experimental reaction rates. Experimental reaction rates were compared with calcula1tion of MCNPX code.

Thesis (MSc)--Stellenbosch University, 2005. / Some digitised pages may appear illegible due to the condition of the original hard copy. / ENGLISH ABSTRACT: Airborne gamma-ray spectrometry is used for exploration and environmental monitoring over large areas. Such datasets of 7-ray are acquired using large 16l NaI(T1) detector crystals mounted in an aircraft. The response of these detectors to naturally occurring radioactive isotopes is a function of detector volume, efficiency and resolution. This response is modelled using the Monte Carlo method. A photon-electron transport computer code, NIPET, is written to calculate the intrinsic efficiency and photofraction of these large prismatic crystals. The intrinsic efficiency indicates the number of incident photons that interact in some way with the detector resulting in a deposition of energy in the crystal. The photofraction, on the other hand, indicates how many of these photons that impinge on the detector are actually recorded with their full initial energy. This study presents explicity calculated photofraction values for 16l NaI(Tl) crystals. Comparison of these new values, calculated with this computer program, with that of published values for small 3" x 3" crystals shows good agreement. However, for large crystals, the calculated values differ from those in the literature by almost 15%. The study also finds that for the gamma-ray energy range between 0.2 - 3.0 MeV, these detectors have an intrinsic efficiency above 90%, whereas the photofraction values range from 80% for low energy photons to above 40% for high energy photons in the case of large crystals. / AFRIKAANSE OPSOMMING: Lug gamma-straal spektroskopie is nuttig vir eksplorasie en omgewings ondersoeke oor groot areas. Metings word tipies gedoen met 16l NaI(T1) detektors wat monteer is in ’n vliegtuig. Die respons van hierdie detektors ten opsigte van natuurlike radioaktiewe isotope is ’n funksie van detektorvolume, doeltreffendheid en oplosvermoë. Hierdie respons word gemodeleer deur gebruik te maak van ’n Monte Carlo tegniek. ’n Rekenaarprogram, NIPET, is geskryf om die intrinsieke doeltreffendheid en fotofraksie vir hierdie groot prismatiese kristalle te bereken. Die intrinsieke doeltreffendheid dui die breukdeel van die invallende fotone aan wat ’n interaksie ondergaan binne die detektor kristal en sodoende energie deponeer. Die fotofraksie, daarenteen, dui die breukdeel invallende fotone aan wat absorbeer word deur die kristal met hul voile invallende energie. In hierdie tesis word eksplisiete fotofraksiewaardes vir 16l NaI(T1) kristale bereken. Goeie ooreenstemming word gevind tussen fotofraksie waardes bereken met hierdie program en die waardes gepubliseer in die literatuur vir klein 3" x 3" kristalle. Vir groter kristalle is daar egter swakker ooreenstemming. Berekende fotofraksie waardes verskil met 15% van die waardes in die literatuur. Daar word ook bevind dat vir gamma-energie tussen 0.2 - 3.0 MeV, die intrinsieke doeltreffendheid vir hierdie tipe detektors bo 90% is en dat fotofraksiewaardes wissel tussen 80% vir lae energie tot bo 40% vir hoë foton energie.

Oito blocos transportáveis para calibração foram construídos para serem utilizados como padrões de concentração na calibração de espectrômetros gama portáteis e aerotransportados. Todo o procedimento de construção é descrito em detalhe. Os blocos, com dimensões de 1 m x 1 m x 0,30 m e massas variando entre 593 kg e 673 kg, devem a sua radioatividade à adição de diferentes quantidades de feldspato potássico (ortoclásio), caldasito e areia monazítica à massa de concreto. As concentrações de potássio, urânio e tório variam significativamente de um bloco para outro atingindo valores máximos de 5,7% de K, 45,6 ppm eU e 137 ppm eTh. A distribuição do fluxo de radiação gama proveniente da superfície dos blocos de concreto e a magnitude das heterogeneidades na concentração dos elementos radioativos foi determinada experimentalmente. Como exemplo de aplicação apresenta-se o resultado da calibração de um espectrômetro gama portátil. / Eight transportable calibration pads were built in to be used as concentration standards for portable and airborne gamma spectrometers calibrations. The pads construction procedure is described in full detail. The pads, with dimensions of 1 m x 1 m x 0,30 m and masses between 593 kg and 673 kg were made radioactive by the addition of different amounts of k-feldspar, caldasite and monazitic sand to the concrete masses. The potassium, uranium and thorium concentration vary significantly in the pads, reaching maximum values of 5,7% of K, 45,6 ppm eU and 137 ppm eTh. The distribution of the gamma radiation flux from the pads surfaces and the heterogeneity magnitudes of the radioactive elements concentration were experimentally established. An example of gamma spectrometer calibration is presented.