2-D reconstruction of elemental distribution within a sample using neutron capture prompt gamma-rays

The technique of emission tomography employing neutron capture prompt gamma-rays is described. Experiments have been carried out to demonstrate this technique employing a high flux reactor neutron beam using an HPGe detector and a scanning system which incorporates a BBC microcomputer for control, data acquisition, image reconstruction and display. Neutron tomography of the same object was also performed in order to correct the emission tomography results for the neutron flux depression within the sample. The images produced represent the intensity of the induced gamma-ray of interest, and hence the concentration of the isotope of interest.     

Elemental analysis of biological matrices using tomographic techniques

Gamma-ray transmission tomography and neutron induced gamma-ray emission tomography (NIGET) where delayed gamma-rays from an activated sample are detected in a tomographic mode, were used to investigate the elemental composition and distribution of a salivary gland stone, nondestructively. Transmission tomography provided information about the distribution of the linear photon attenuation coefficient in the object and showed clearly the two regions of inorganic and organic material in a number of sections through it. In addition it was possible to derive from the data the concentration of Ca and the ratio of Ca to P in the stone. By using NIGET it was shown that the concentration of Ca and Na in the object can be mapped and quantitative measurements of these elements could be obtained in any particular location within the salivary gland stone. The spatial resolution which depends on detector collimation was 1 mm for transimission and 2 mm for emission measurements. Instrumental neutron activation analysis was also used to determine the concentration of five elements in the stone, as a whole.     

A new NaI detector arrangement for efficient detection of high energy gamma-rays

Summary Prompt gamma-ray neutron activation analysis (PGNAA) and neutron inelastic scattering (NIS) techniques have been widely used for measuring elemental composition in bulk samples. The neutrons and gamma-rays used in this technique are highly penetrating, which allows the analysis of large sample volumes. In the oil well logging industry, there are limitations on the size of detectors used -particularly the detector diameter. This limitation can lead to a low detection probability for the high energy gamma-rays. A new NaI detector arrangement (patent pending) has been designedto deal with this problem. The arrangement consists of two NaI detectors, one of which is a well type. The first detector is 1"×5" and the second is a well type 5" long with a wall thickness of 0.35" and a hole diameter of one inch. The first detector is placed inside of the well detector for use. Feasibility studies were performed with this arrangement using a ²⁴Na radioactive source and a sulfur sample or prompt gamma-rays. An enhancement in the signal-to-noise ratio (SNR) was observed in both cases based on the peak height to continuum height in the resulting prompt gamma-ray spectra.     

A dual purpose Compton suppression spectrometer

A gamma-ray spectrometer with a passive and an active shield is described. It consists of a HPGe coaxial detector of 42% efficiency and 4 NaI(Tl) detectors. The energy output pulses of the Ge detector are delivered into the 3 spectrometry chains giving the normal, anti- and coincidence spectra. From the spectra of a number of ¹³⁷Cs and ⁶⁰Co sources a Compton suppression factor, SF and a Compton reduction factor, RF, as the parameters characterizing the system performance, were calculated as a function of energy and source activity and compared with those given in literature. The natural background is reduced about 8 times in the anticoincidence mode of operation, compared to the normal spectrum which results in decreasing the detection limits for non-coincident gamma-rays up to a factor of 3. In the presence of other gamma-ray activities, in the range from 5 to 11 kBq, non- and coincident, the detection limits can be decreased for some nuclides by a factor of 3 to 5.7.     

Prompt Gamma Neutron Activation Analysis of 316-L Stainless Steel

Prompt gamma-rays from thermal neutron capture reaction have been used to measure the concentrations of the main constituents namely Fe, Ni and Cr in 316-L stainless steel using recently established prompt gamma neutron activation analysis (PGNAA) facility at Pakistan Institute of Nuclear Science and Technology (PINSTECH). High resolution, high purity germanium detector with 40% relative efficiency was employed for the gamma-ray spectroscopy of the samples. The interference-free full energy gamma-ray peaks of the elements of interests were selected in the high energy low background region (5.0–9.0 MeV). The efficiency calibration of the detector was performed using ultra pure standards of chromium and chlorine obtained respectively from Merck and Alpha Inorganics. This paper describes, in addition, the salient features as well as the background of establishing PGNAA facility at the Institute.     

The application of NAA with irradiation at reduced temperature for the study of element losses during pretreatment of biological samples

The neutron capture gamma-ray spectroscopy facility assembled at the Institute of Radiochemistry, KfK (for analytical purposes) using a²⁵²Cf neutron source with a strength of 6·10⁷ n/s, has been used to check its applicability and sensitivity for quantitative analyses of ores. The analysis of Sm, Cd and Mn in phosphate and monazite rock samples has been carried out. The results from this study show a variation of about 25% from the values determined by RNAA method. This discrepancy could be mainly due to the low signal-to-background ratio observed which is caused by (i) scattering of the source gammarays by the target, and (ii) interference from the 2223.1 keV neutron capture hydrogen gamma-rays produced by the moderated materials and from their compton scattering in the detector. To overcome these difficulties we suggest to introduce a 2.5 cm thick polyethylene sheet between the detector⁶Li-cap shielding and the target as well as to increase the detection solid angle. Also the strength of the²⁵²Cf neutron source should be increased by an order of magnitude and the neutron beam should be collimated to obtain the optimal thermal neutron flux with a low level of²⁵²Cf gamma-rays. This can be achieved by setting up between the neutron source and the target a conical polyethylene collimator with a thickness of 10 cm containing a 1 cm thick lead sheet.     

Compton suppression system at Penn State Radiation Science and Engineering Center

A Compton suppression system is used to reduce the contribution of scattered gamma-rays that originate within the HPGe detector to the gamma-ray spectrum. The HPGe detector is surrounded by an assembly of guard detectors, usually NaI(T1). The HPGe and NaI(T1) detectors are operated in anti-coincidence mode. The NaI(T1) guard detector detects the photons that Compton scatter within, and subsequently escape from the HPGe detector. Since these photons are correlated with the partial energy deposition within the detector, much of the resulting Compton continuum can be subtracted from the spectrum reducing the unwanted background in gamma-ray spectra. A commercially available Compton suppression spectrometer (CSS) was purchased from Canberra Industries and tested at the Radiation Science and Engineering Center at Penn State University. The PSU-CSS includes a reverse bias HPGe detector, four annulus NaI(T1) detectors, a NaI(T1) plug detector, detector shields, data acquisition electronics, and a data processing computer. The HPGe detector is n-type with 54% relative efficiency. The guard detectors form an annulus with 9-inch diameter and 9-inch height, and have a plug detector that goes into/out of the annulus with the help of a special lift apparatus to raise/lower. The detector assembly is placed in a shielding cave. State-of-the-art electronics and software are used. The system was tested using standard sources, neutron activated NIST SRM sample and Dendrochronologically Dated Tree Ring samples. The PSU-CSS dramatically improved the peak-to-Compton ratio, up to 1000:1 for the ¹³⁷Cs source.     

Multiple gamma-ray detection method and its application to nuclear chemistry

A new radionuclide quantification method is proposed on the basis of multiple gamma-ray detection, which is two or higher fold gamma-ray coincidence method. The coincidence method has so far been used for nuclear structure study. We apply this method for quantification of radioactive nuclei. The advantage of this method consists of high energy resolution and high sensitivity. It is successfully applied to nuclear waste analysis, neutron activation analysis and prompt gamma-ray analysis. The principle of the multiple gamma-ray detection method and future perspectives for an innovative pulsed neutron source and a new detector system will be presented.     

Preparation and Pharmacokinetic Evaluation of Iodine-125 Labeled Alphamethyl-L-Tyrosine

A prompt gamma-ray neutron activation analysis (PGNAA) system was used to calibrate and validate a Monte Carlo model as a proof of principle for the quantification of chlorine in soil. First, the response of an n-type HPGe detector to point sources of ⁶⁰Co and ¹⁵²Eu was determined experimentally and used to calibrate an MCNP4a model of the detector. The refined MCNP4a detector model can predict the absolute peak detection efficiency within 12% in the energy range of 120–1400 keV. Second, a PGNAA system consisting of a light-water moderated ²⁵²Cf (1.06 g) neutron source, and the shielded and collimated HPGe detector was used to collect prompt gamma-ray spectra from Savannah River Site (SRS) soil spiked with chlorine. The spectra were used to calculate the minimum detectable concentration (MDC) of chlorine and the prompt gamma-ray detection probability. Using the ²⁵²Cf based PGNAA system, the MDC for Cl in the SRS soil is 4400 g/g for an 1800-second irradiation based on the analysis of the 6110 keV prompt gamma-ray. MCNP4a was used to predict the PGNAA detection probability, which was accomplished by modeling the neutron and gamma-ray transport components separately. In the energy range of 788 to 6110 keV, the MCNP4a predictions of the prompt gamma-ray detection probability were generally within 60% of the experimental value, thus validating the Monte Carlo model.     

Coincidence and anti-coincidence measurements in prompt gamma neutron activation analysis with pulsed cold neutron beams

A novel approach is implemented to alleviate some persistent problems in neutron capture prompt gamma activation analysis (PGAA). Detection sensitivities of PGAA are often restricted by the following factors: poor signal to noise ratios, interferences from background signals, and, in some cases, overlapping energy lines from different origins, namely ultra short-lived decay lines interfering with prompt decay. Timing the gamma-ray acquisition with the actual capture events using a pulsed beam of cold neutrons allows discrimination between prompt and delayed emissions from a sample source as well as against background events. Coincidence gating selects the prompt gamma-ray emissions. Contributions of background capture gamma-rays are suppressed because of different flight times of neutrons to the sources of background radiation, providing a reduction in direct gamma-ray interferences. Anti-coincidence gating allows measurement of only decay radiation that originates from short-lived activated states of the nuclides after capture. Spectra of decaying nuclides are free of interfering prompt activities, as well as have lower continuum background from Compton scattering of high-energy prompt gamma-rays in the detector. The measurements provide the opportunity to use ultra-short half-life nuclides for analytical purposes, no sample transfer times are lost, and repetitive activation and counting cycles are achieved with the use of pulsed neutron beams.     

Prompt Gamma-Ray Activation Analysis: Fundamentals and Applications

Prompt gamma-ray activation analysis (PGAA) is an important nuclear analytical technique that complements conventional neutron activation analysis (NAA). When a target is placed in a beam of neutrons, gamma-rays emitted upon neutron capture are measured by a shielded germanium detector, yielding quantitative elemental analysis. The radiation is penetrating and the analysis both nondestructive and independent of the chemical form of the element(s) being measured. The technique is most useful for measurement of light elements (H, B, C, N, Si, P, S, Cl) which can not be easily measured by other methods. Best sensitivity is achieved with neutron beams from research reactors. Although sample preparation is minimal, care must be taken to select proper standards and blanks, and numerous corrections must sometimes be applied to the data from the complex spectra. PGAA has proven useful for multielement analysis of a wide variety of different materials spanning a broad range of scientific disciplines. Of particular importance has been the measurement of hydrogen in materials.     

Development of a neutron beam line and detector system for multiple prompt gamma-ray analysis

A neutron beam line for multiple prompt gamma-ray analysis was constructed at the Japan Atomic Energy Agency. A detector system for the MPGA was constructed at the C2-3-2 beam line in January 2005. It comprised eight (upgraded in March 2007) clover Ge detectors with a BGO Compton suppressor. High efficiency detector system provides an advantage in terms of the detection limit of MPGA when compared to the result of PGA. The supermirror neutron bender was improved and a supermirror neutron guide was installed upstream of the sample position.     

Evaluation of an alternative convenient irradiation system for determination of emission rate of radio-isotopic neutron sources

In present work, an alternative irradiation system based on a symmetric cylindrical tank filled with a moderator containing hydrogen, which was equipped with a NaI(Tl) scintillation detector, was proposed for using in determination of neutron flux. This irradiation system was designed by MCNP4C code, with considering a ²⁴¹Am–Be neutron source in several volumes and different materials. When the neutron is captured by hydrogen, a 2.22 MeV prompt gamma-ray is emitted. The gamma pulse-height spectrum shows a photo-peak around 2.22 MeV whose net area is proportional to the total emission rate of neutron. The simulation result showed that a cylindrical tank with 110 cm diameter and height filled with water can be a suitable system for neutron source strength calibration. Furthermore, a proper two-layer shielding must be placed between the source and detector for preventing neutrons and gamma rays to directly enter the detector.     

The Compton continuum: Nuisance or new information in NAA?

The Compton continuum in large sample neutron activation analysis has a measurable contribution from scattering of gamma-rays in the sample itself besides from scattering in the detector. The continuum, therefore, contains information on the sample’s composition, which may be made available by chemometrics. This hypothesis was tested on four types of animal fodder with similar amounts of mineral supplements. First results indicate indisputable discrimination of the sample types if using peakless parts of the gamma-ray spectra of the natural radioactivity of the materials as well as of those obtained after neutron activation of 1 kg samples. It indicates that the valuable information on differences in, e.g., organic constituents may be obtained by analyzing the Compton continuum.     

{\rtf1\ansi\ansicpg1250\deff0\deflang1038\deflangfe1038\deftab708{\fonttbl{\f0\froman\fprq2\fcharset238{\*\fname Times New Roman;}Times New Roman CE;}} \viewkind4\uc1\pard\f0\fs24 Status of software for PGNAA bulk analysis by the Monte Carlo - Library Least-Squares (MCLLS) approach \par }

Summary {\rtf1\ansi\ansicpg1250\deff0\deflang1038\deflangfe1038\deftab708{\fonttbl{\f0\froman\fprq2\fcharset238{\*\fname Times New Roman;}Times New Roman CE;}} \viewkind4\uc1\pard\f0\fs24 The Center for Engineering Applications of Radioisotopes (CEAR) has been working for about ten years on the Monte Carlo - Library Least-Squares (MCLLS) approach for treating the nonlinear inverse analysis problem for PGNAA bulk analysis. This approach consists essentially of using Monte Carlo simulation to generate the libraries of all the elements to be analyzed plus any other required libraries. These libraries are then used in the linear Library Least-Squares (LLS) approach with unknown sample spectra to analyze for all elements in the sample. The other libraries include all sources of background which includes: (1) gamma-rays emitted by the neutron source, (2) prompt gamma-rays produced in the analyzer construction materials, (3) natural gamma-rays from K-40 and the uranium and thorium decay chains, and (4) prompt and decay gamma-rays produced in the NaI detector by neutron activation. A number of unforeseen problems have arisen in pursuing this approach including: (1) the neutron activation of the most common detector (NaI) used in bulk analysis PGNAA systems, (2) the nonlinearity of this detector, and (3) difficulties in obtaining detector response functions for this (and other) detectors. These problems have been addressed by CEAR recently and have either been solved or are almost solved at the present time. We have now finished the development of Monte Carlo simulation for all of the libraries except the prompt gamma-ray library from the activation of the NaI detector. We must first determine a treatment for the coincidence schemes for Na and particularly I to complete the Monte Carlo simulation of this last library. \par }     

Multiple prompt gamma-ray analysis and construction of its beam line

By combining neutron activation analysis with multiple gamma-ray detection (gamma-gamma coincidence), we have proved better sensitivity and resolution for the trace element analysis than the ordinary single gamma-ray detection method. We now try to apply the multiple gamma-ray detection method to the prompt gamma ray analysis (PGA). We have established a new cold neutron beam line for PGA in Japan Research Reactor, JRR-3M, at Tokai establishment of Japan Atomic Energy Research Institute (JAERI). It consists of a beam shutter, a beam attenuator, a gamma-ray detector array, a sample changer, and a beam stopper. We construct a high-efficiency gamma-ray detector array specially designed for this purpose. Its performance has been evaluated with the Monte Carlo simulation code, GEANT 4.5.0.     

Prompt and delayed radiation measurements in the elemental analysis of biological materials: The case for neutron induced gamma-ray emission tomography

Nuclear and atomic methods of analysis, which rely on the detection of prompt and delayed radiations, emitted as a result of interactions between radiation probe and target, for determining the elemental concentration in vivo and in vitro, are summarily reviewed, with reference to bone analysis; the demand for methods which provide information about elemental distribution is highlighted. The way neutrons can be used as probes to investigate the composition and structure of objects by employed the principles of computerised tomography are outlined and the novel modes of utilisation are briefly described: neutron transmission tomography, neutron induced prompt gammaray emission tomography and neutron induced delayed gamma-ray emission tomography. The latter method, alternatively termed neutron activation tomography, is then used to determine on-destructively the distribution of Na in selected planes of a human tibia, in vitro, by measuring the activity of²⁴Na using a NaI(Tl) and a Ge(Li) detector in a tomographic scanner which incorporates a microcomputer for control, data acquisition and image reconstruction. The problems of attenuation and scattering are discussed as are the limitations for quantitative results of this useful new mode of tomography which provided information about composition and elemental distribution in a material.     

Improved radioxenon gamma-spectrometry counting system and its efficiency calibration: Monte Carlo simulation and experimental results at enriched xenon counting environment

To give satisfactory efficiency both for X- and gamma-ray photon, an improved counting system has been developed in CTBT Canadian radioxenon laboratory. The counting system consists of a BEGe detector coupled with a thin carbon fiber window counting cell, that can perform a reliable and efficient radioxenon measurement. A semi-empirical calibration procedure was adopted, which is a combination of experimental measurement and mathematical simulation. Mathematical calibration tool is Monte Carlo simulation software named VGSL. Advanced gamma-spectrum analysis software, named Aatami, was used for gamma-ray peak shape fitting and X-ray multiplets deconvolution. The calculated full energy peak efficiency curve covers from 30 to 700 keV and agrees well with experimental data points within 2%. The efficiency curve can provide radioxenon analysis both for X-rays and gamma-rays with high quality. The efficiency distortion near xenon k-absorption edge of 35 keV, which is caused by high concentrated xenon in the counting cell, is also discussed.     

Measurement of k0-Factors in Prompt Gamma-Ray Neutron Activation Analysis

The guided thermal neutron beam at 100 MW Dhruva research reactor facility of Bhabha Atomic Research Centre (BARC) was used to carry out prompt gamma-ray neutron activation analysis (PGNAA). The prompt k ₀-factors have been determined for the isotopes of the elements H, B, K, Co, Cu, Ca, Ti, Cr, Cd, Ba, Hg and Gd with respect to 1951 keV gamma-line of ³⁶Cl. The prompt k ₀-factors for H, Cl and Cu were also measured with respect to the 1381 keV gamma-line of ⁴⁹Ti. Different samples like NH₄Cl, Ti metal, cobalt chloride and other stoichiometric compounds and pure metals were used for this purpose. Prompt gamma-rays were accumulated using a 22% HPGe detector connected to a PC based 8k MCA in single mode counting. The energy calibration in the range of 100–8500 keV was carried out using gamma-rays from ¹⁵²Eu and ⁶⁰Co, and the prompt gamma-rays from ³⁶Cl whereas the absolute detection efficiency for this energy range was determined using ¹⁵²Eu and prompt gamma-rays from ³⁶Cl and ⁴⁹Ti.     

Non-destructive assay technique for the determination of <Superscript>238</Superscript>U/<Superscript>232</Superscript>Th ratio in the mixed oxides of uranium and thorium using prompt gamma-ray neutron activation

A non-destructive assay technique based on prompt gamma-ray neutron activation analysis for the determination of ²³⁸U to ²³²Th ratio in the mixed oxide fuel materials has been established. The method uses closely spaced high energy gamma-rays in the region of 4000 keV to 4150 keV enabling it to be applied for samples of any geometry and thickness without having any correction for gamma-ray attenuations and detection efficiencies.