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.     

Analysis of toxic elements by MPGA

In order to improve the sensitivity for the quantification of trace elements, we propose the combination of prompt gamma-ray analysis (PGA) and a multiple gamma-ray detection method. A new Ge detector system for multiple prompt gamma-ray analysis (MPGA) was constructed at the neutron guide-hall of the JRR-3M reactor of the Japan Atomic Energy Agency (JAEA). The first demonstration of this system was given with a plastic sample containing traces of cadmium. The quantification limit of cadmium in a plastic sample was found to be about 0.1 ppm.     

Determination of As and Sb in iron and steel by neutron activation analysis with multiple gamma-ray detection

Recycled steel products demands a new technique for determining tramp elements in steel. In this paper, As and Sb in iron certified reference materials were determined by neutron activation analysis with the multiple gamma-ray detection method. The determined values are in good agreement with certified and reference values. The lower determination limits (LDL) for As and Sb in high purity iron are 0.012 and 0.0025 ppm, respectively. As the demanded LDL for As and Sb is 0.1 ppm, the method described in this work is suitable for determining As and Sb in recycled steel.     

Performance evaluation of spectral deconvolution analysis tool (SDAT) software used for nuclear explosion radionuclide measurements

The Spectral Deconvolution Analysis Tool (SDAT) software was developed to improve counting statistics and detection limits for nuclear explosion radionuclide measurements. SDAT utilizes spectral deconvolution spectroscopy techniques and can analyze both β-γ coincidence spectra for radioxenon isotopes and high-resolution HPGe spectra from aerosol monitors. Spectral deconvolution spectroscopy is an analysis method that utilizes the entire signal deposited in a gamma-ray detector rather than the small portion of the signal that is present in one gamma-ray peak. This method shows promise to improve detection limits over classical gamma-ray spectroscopy analytical techniques; however, this hypothesis has not been tested. To address this issue, we performed three tests to compare the detection ability and variance of SDAT results to those of commercial-off-the-shelf (COTS) software which utilizes a standard peak search algorithm.     

Lower limit of determination values for trace elements in iron certified reference materials by neutron activation analysis with multiple gamma-ray detection

Recycling steel products demands a new technique for determining tramp elements in steel. Tramp elements, As and Sb, in some iron certified reference materials were determined by neutron activation analysis with multiple gamma-ray detection method and reported in MTAA11. In MTAA12, the authors reported the lower limit of determination values (LDL) and the dispersion of this method. The values of the LDLs for As and Sb in high purity iron were 0.002 and 0.0009 μg·g⁻¹. The dispersion is small enough to satisfy the demand from materials science.     

First Results from the Prompt Gamma-Ray Activation Facility at PSI

Since October 1997, a new Prompt Gamma-ray Activation (PGA) Facility at the neutron spallation source SINQ of the Paul Scherrer Institute (PSI) in Villigen in Switzerland has been operational. The detection system includes a Compton-suppression and a pair spectrometer. Of particular interest is the availability of a neutron focusing lens. During the beam periods 1997 and 1998, measurements were performed to characterize the PGA facility (gamma-ray background, profile and flux of the neutron beam, efficiencies of the two spectrometers, analytical sensitivities and detection limits for several elements, elemental analysis of standards). Scanning of samples and nuclear spectroscopy of isotopes having small capture cross section were also performed using the neutron focusing lens.     

Design of a new instrument for cold neutron prompt gamma-ray activation analysis at NIST

A new instrument for cold neutron prompt gamma-ray activation analysis (CNPGAA) is being designed and constructed at the NIST Center for Neutron Research (NCNR). The new instrument is expected to have lower gamma-ray and neutron background and better detection limits for most elements than the current cold neutron PGAA instrument. Other advantages over the current facility will include the ability to analyze larger samples and greater overall measurement capability due to the addition of scanning stages, cryostats, and sample changers.     

Parameterization of detector efficiency for the standardization of NAa with stable low flux reactors

With SLOWPOKE and MNS reactors which have reproducible neutron fluxes, the standardization of multielement NAA can be reduced to measuring activation constants once for all elements and then determining relative detection efficiencies for new detectors and counting geometries. In this work, a method has been developed for the parameterization of the efficiency of gemanium detectors. The gamma-ray detection efficiency was measured as a function of energy and distance for three detectors. The variation with distance was found to follow a modified EID law, within 1%, for point sources 1 mm to 250 mm from the detector. A model, including coincidence summing corrections, was developed to calculate efficiency for NAA samples; it requires 16 measured parameters. Tests showed that the calculated relative detection efficiencies are accurate to better than 3% for close counting geometries and sample volumes up to a few millilitres. Areas of possible improvement to the accurarcy of the method are suggested.     

Optimization of HANARO cold neutron induced prompt gamma activation analysis system by using Monte Carlo code

Prompt gamma activation analysis (PGAA) is a nuclear analytical technique for non-destructive determination of elemental and isotopic compositions. The principle of PGAA technique is based on detection of captured gamma-ray emitted from an analytical sample while being irradiated with neutrons. Use of a cold neutron beam guide greatly reduces the gamma-ray background at the analytical sample while maintaining a neutron capture rate is comparable to that of standard thermal neutron PGAA. A new cold neutron induced prompt gamma activation analysis (CN-PGAA) system has been under construction since April of 2009 at the HANARO Cold Neutron Building (KAERI, Republic of KOREA). In this study, the Compton suppression factor of the CN-PGAA system was estimated to be 5.5 using a ⁶⁰Co radioactive source in conjunction with the MCNPX simulations. Several parameters of the CN-PGAA system were studied to estimate and optimize the performance of the system: scintillation material in the guarded detector of a Compton suppression spectrometer (CSS); the relative positions of the HPGe detector and annular detector; and the distance between the HPGe detector and back catcher BGO detectors of the CSS. In addition, the neutron ray-trace simulation package, McStas, was adopted to predict the neutron flux and wavelength distribution at the end of the cold neutron beam guide. These results served as input for the MCNPX simulation of the CN-PGAA system.     

Coincidence counting for PGNAA applications: Is it the optimum method?

Summary One of the main advantages of γ-γ coincidence counting is the reduction of the background spectrum, pulse pile-up, and summing effects (for simple schemes). For prompt gamma-ray neutron activation analysis (PGNAA), the sources of background include the gamma-rays from the natural background, from surrounding materials, from the neutron source, and from detector neutron activation. While this counting approach effectively increases the signal-to-noise (S/N) ratio, it also decreases the signal counting rate. This adds some practical limitations to using this approach. In this work, two examples are presented for the efficient use of the coincidence counting approach.     

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.     

Improvements of neutron activation techniques for the determination of fissile material concentrations

Certain experimental improvements, as variable sample size and irradiation position, automation and flexibility in radiation detection, broaden the measurable concentration range, increase the possible rate and accuracy of analysis and enlarge the application range of the home-made nuclear analyzer for fissile material analysis by delayed fission neutron counting and for short-lived multielement analysis by neutron activation gamma-ray spectrometry. Intercomparisons of results by various methods and laboratories show the need for regular checks of techniques to ensure reliable measurements.     

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.     

Determination of the elemental distribution in a sample using neutron induced gamma-ray emission tomography

The factors that affect accurate, quantitative results to be obtained by neutron induced gamma-ray emission tomography are stated. The technique, which is a combination of neutron activation analysis with computerised gamma-ray emission tomography, would be enhanced by the use of multiple detector assemblies, in geometrical configurations, which simultaneously record the gamma-rays emitted and improve detection efficiency. Developments in the past few years in positron emission tomography (PET) where scanners made of single scintillation block detectors, cut into smaller segments, to form individual crystal detector elements and packed in ring around the radioactive object, are discussed. The coincident detection efficiency for annihilation photons and cascade gamma-rays for such systems are considered and the possibilities of carrying out NIGET with coincident gamma-ray tomography are explored whilst indicating some of the limitations. This is an area which requires further, intense investigation and has an impact on a wide range of applications, particularly in the biomedical field.     

Application of multiple prompt gamma-ray analysis (MPGA) to geochemical and cosmochemical samples

A prompt gamma-ray analysis system using multiple detection method (MPGA system) was constructed at the neutron guide hall of the JRR-3M reactor of the Japan Atomic Energy Agency. We applied MPGA method to geochemical and cosmochemical samples to evaluate its analytical performance on signal to noise (S/N) ratio, sensitivity, and detection limit. The S/N ratio measured by MPGA system was larger than that by normal prompt gamma ray activation analysis (PGAA) at JRR-3M. For some elements, the S/N ratio was improved more than ten times. Several elements that are not detected by PGAA were detected by MPGA. At the present time, concentrations of major elements and trace elements with high neutron capture cross section in geochemical and cosmochemical samples were determined accurately by the MPGA system installed at JRR-3M. It is expected that it will determine a lot of trace elements after appropriate adjustments and modifications.     

Determination of gold in biological materials by radiochemical neutron activation analysis

A radiochemical neutron activation analysis procedure was developed for the determination of trace amounts of gold in biological materials. The procedure was realized with irradiation of reference and test samples in a nuclear reactor, selective and quantitative separation of gold using inorganic MnO₂ Resin and gamma-ray spectrometric measurement of ¹⁹⁸Au. The method is characterized by a low limit of detection of gold at ng g^?1 level. Results shows that the method can be applied to the determination of trace amounts of gold in tissues for medical research.     

A multiple time-gated system for pulsed digital gamma-ray spectroscopy

Neutron activation analysis (NAA) systems that use pulsed neutron generators (NGs) employ spectrum gating procedures to segregate nuclear processes by acquiring gamma-ray spectra separately when the generator is on (HIGH gate) and off (LOW gate). Often, the actual neutron burst lags the leading edge of the HIGH gate signal by a few μs. Thus, count rates vary not only between the on and off states of the NG, but within them as well. Recent advances in digital gamma-ray spectrometers that allowed the concurrent acquisition of data by sorting events into two separate spectra based on gate status suggested that a time-resolved analysis that further subdivided the neutron pulse cycle could obtain further information to separate gamma-rays produced by different nuclear reactions. In this paper we introduce a gating system for time-resolved NAA that is capable of concurrently acquiring as many as 16 spectra from up to 8 user-defined time intervals during each of the HIGH gate and LOW gate periods, each with all required timing and count rate information. We present the new gating system’s implementation, operation and some first experimental test results.     

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.     

Cold neutron facility for prompt gamma-neutron activation analysis

The restart of the recently upgraded research reactor in Budapest is foreseen at the end of this year. A number of fast, thermal and cold neutron beams will serve for research, industrial and educational activities. One of the cold neutron guide end positions will be utilized for neutron capture prompt gamma-ray activation analysis (PGAA). Further development of the PGAA method as well as new applications in environmental research, biology and medicine are planned.     

Non-destructive compositional analysis of sol–gel synthesized lithium titanate (Li2TiO3) by particle induced gamma-ray emission and instrumental neutron activation analysis

Lithium titanate, one of the important tritium breeding materials in D–T based fusion reactor under ITER programme, was synthesized through sol–gel route. For chemical quality control of finished product, it was necessary to quantify the lithium and titanium contents. As this ceramic sample is difficult to dissolve, non-destructive analytical methods are preferred for compositional analysis. In the present work, two non-destructive nuclear analytical methods namely particle induced gamma-ray emission (PIGE) using proton beam and instrumental neutron activation analysis (INAA) using reactor neutrons were standardized for the determination of lithium and titanium concentrations, respectively and applied to eleven samples of lithium titanate. To the best of our knowledge, Li quantification in lithium titanate sample is being reported for the first time using PIGE. For quantifications of Li and Ti, 478 keV prompt gamma-ray from ⁷Li (p, p′γ) ⁷Li and 320 keV gamma-ray from ⁵⁰Ti (n,γ) ⁵¹Ti were measured, respectively, by high resolution gamma-ray spectrometry. The PIGE and INAA methods were validated using several synthetic samples containing lithium and titanium, respectively. Concentrations of lithium and titanium and Li/Ti mole ratios were evaluated and compared with the stoichiometric concentration of Li₂TiO₃.