The McMaster University Nuclear Reactor (MNR) research facilities

The McMaster University Nuclear Reactor (MNR) is a unique Canadian facility in a university environment welcoming researchers from across Canada and abroad. The irradiation and analytical facilities available cover a broad spectrum of nuclear analytical techniques from standard INAA to fully automated counting systems for prompt gamma activation analysis and delayed neutron counting. In addition, neutron beams provide for a wide spectrum of applied and basic nuclear research applications. This paper describes the state-of-the-art facilities available at McMaster.     

The upgrading of the cyclic neutron activation analysis facility at the Dalat research reactor

Journal of Radioanalytical and Nuclear Chemistry - The cyclic neutron activation analysis (CNAA) facility based on a pneumatic transfer system for short irradiation and rapid counting has recently...     

NADA: A versatile PC based program for neutron activation data analysis

We have developed a PC based program for neutron activation data analysis using the FORTRAN and C languages. The routines are based on creating files associated with conventional ORTEC hardware and output software. The main features of the program include radionuclide identification, and the use of semi-automatic integration or the peak fitting SAMPO routine. Other developments are hard and soft copy records for detailed sample identification and particular irradiation, decay and counting procedures. Flux variations, high deadtime corrections, counting geometries, spectral and nuclear interferences, as well as uranium fission interferences are also automatically accounted for. The data output includes concentration values in %, ppm, g or ppb units with associated errors, while detection limits for each individual sample are indicated. Further data output can easily be generated which can be imported to most spreadsheet programs for various statistical uses. A future implementation to the program will include batch-file processing and automated self-absorption calculations for geological samples.     

Activation analysis with standards containing two or more active nuclides A computerized method of calculation involving decay and gamma spectral resolution

The resolution of the gamma spectra of activities induced in materials by fast neutron, charged particle and gamma photon activation is complicated by the fact that many elements produce more than one active nuclide in significant amounts. Direct resolution by least-squares fitting of the spectra of standards is only possible in these circumstances if the standard and sample spectra are obtained at the same time after irradiation, as the shapes of the standard spectra change with time. An alternative to the practical collection of spectra in this way is the correction of the standard spectra to the mid-time of counting of a sample spectrum. This may be achieved by recording spectra for a standard at different times and resolving the decay curves obtained for each channel on the basis of the half-lives of the component nuclides, which may be decay-independent or related or both. From the component nuclide count-rates in each channel at some arbitrary time, the standard spectrum at the time of counting of the sample can be generated and then used in a conventional least squares-fit of the sample spectrum. A FORTRAN IV program has been written to carry out this type of calculation on an IBM 360 65 computer. The feasibility of using this method is demonstrated by its application to activation analyses involving standards containing decay-related and independent nuclides.     

Evaluation of concentrations of major and trace elements in human lung using INAA and PIXE

The elemental concentrations of Br, Ca, Ce, Cl, Co, Cr, Cs, F, Fe, Hf, K, Mg, Mn, Na, O, Rb, Sb, Sc, Se, V and Zn in 15 human lung autopsy samples, taken from subjects aged more than fifty years old, were determined by instrumental neutron activation analysis (INAA) using reactor neutrons in conjunction with a high resolution detection system. Two modes of irradiation and counting were applied; namely cyclic neutron activation analysis (CNAA) and conventional neutron activation analysis. Proton induced X-ray emission (PIXE) analysis, using a proton beam emerging from a 2 MV Van de Graff accelerator, was additionally employed and Ge, Ni, P and Ti were also identified in the lung tissue. Detection of the X-ray spectra was performed using a high resolution Si(Li) semiconductor. The relevance of these results, including a comparison between the concentrations of elements measured in a pig's lung using CNAA and those found in the human lung is discussed.     

Neutron activation analysis without multi-element standards

The paper shows how, from the neutron irradiation of multi-element standards, one can derive neutron flux parameters for the irradiation position and, at the same time, greatly improve knowledge of nuclear data parameters, such as thermal cross sections, resonance integrals and gamma raz emission probabilities, for the nuclides concerned. It is then shown how the resulting neutron flux parameters and nuclear data parameters can be used to carry out neutron activation analysis without further irradiation of multi-element standards. The technique is applied to the analysis of Chinese geochemical reference material     

Short-time neutron activation gamma-ray spectroscopy

Short-time instrumental neutron activation analysis, with high throughput, sensitivity and accuracy without matrix interferences, can be achieved in spite of the initial high count rate from both short and long-lived nuclide activation, if the experimental conditions are optimized by the combination of techniques. Thus the initial usually high counting rate can be faced by a loss-free counting system to avoid blocking or distortion of the system. The rapid radioactive decay and the consequent low counting statistics of short lived nuclides can be compensated by source-detector distance variation during the counting period and by cyclic and cumulative activation. Matrix spectral interferences can be reduced by ion exchange before activation for selective element preseparation and by neutron spectrum optimization such as epithermal neutron activation for selective element peak enhancement.     

Short-time neutron activation gamma-ray spectroscopy

Short-time instrumental neutron activation analysis, with high throughput, sensitivity and accuracy without matrix interferences, can be achieved in spite of the initial high count rate from both short and long-lived nuclide activation, if the experimental conditions are optimized by the combination of techniques. Thus the initial usually high counting rate can be faced by a loss-free counting system to avoid blocking or distortion of the system. The rapid radioactive decay and the consequent low counting statistics of short lived nuclides can be compensated by source-detector distance variation during the counting period and by cyclic and cumulative activation. Matrix spectral interferences can be reduced by ion exchange before activation for selective element preseparation and by neutron spectrum optimization such as epithermal neutron activation for selective element peak enhancement.     

Observations relative to epithermal and fast neutrons in INAA

Various theoretical and practical aspects of epithermal neutron activation analysis (ENAA) and fast-neutron-induced reaction interferences in conventional instrumental thermal neutron activation analysis (TNAA) have been considered. A new generalized advantage factor which reflects a practical improvement of detection limits in ENAA is proposed. In the determination of practical advantage factors, consideration is also given to the different irradiation channels available for the experiment in a given reactor, or even in several accessible reactors. Fast neutron reaction interference factors are tabulated for both ENAA and TNAA and examples are given of specific interferences in TNAA for some biological and geological matrices.     

Combining prompt gamma activation analysis and off-line counting

The off-line γ-counting of in-beam activated radionuclides has been explored to extend the detection capabilities of prompt gamma activation analysis (PGAA). Such combination of the prompt measurement with a subsequent decay-counting is feasible if radionuclides with half-lives of minutes or hours are produced in the sample during neutron irradiation. Thanks to the simpler spectrum and the higher counting efficiency of decay counting, both selectivity and sensitivity can be improved. The pros and cons of the proposed method have been demonstrated on a series of industry-related measurements.     

Optimized automated activation analysis

A combination of special techniques has been developed for optimization of experimental conditions in order to improve the analytical capability, to facilitate automation and to broaden the applicability of instrumental neutron activation analysis. The techniques used are: (1) compensation for the rapid radioactive decay of short-lived nuclides with the increase of the counting efficiency by automatic source movement to the detector during the counting period, to minimize count rate variations and to prolong the counting period, (2) repeated cyclic and cumulative activation to improve the counting statistics, (3) instrumental correction of counting losses at high and varying count rates by a loss-free counting system and (4) differentiation of the reactor neutron spectrum to enhance the counts from the nuclides of interest by reducing matrix interferences. By optimized combination and automation of these techniques significant improvement of the capability of instrumental neutron activation analysis can be achieved.     

Development of automated analytical systems for large throughput

The need to be able to handle a large throughput of samples for neutron activation analysis has led to the development of automated counting and sample handling systems. These are coupled with available computer-assisted INAA techniques to perform a wide range of analytical services on a commercial basis. A fully automated delayed neutron counting system and a computer-controlled pneumatic transfer for INAA use are described, as is a multi-detector gamma spectroscopy system.     

Phosphorus determination in milk and bone samples by neutron activation analysis

The determination of phosphorus in milk and bone samples by both radiochemical and instrumental neutron activation analysis is described. The radiochemical method consists of thermal neutron irradiation of samples and standards, sample dissolution, phosphorus precipitation as ammonium phosphomolyb-date, use of zinc holdback carrier and counting of the phosphorus-32 ß-activity. The instrumental method involves thermal neutron irradiation of samples and standards, waiting for a decay time and ß-counting. The methods were applied to commercial samples and reference materials.     

Investigating the antimony determination in environmental samples by NAA

In recent years, environmental concerns regarding antimony have grown considerably due to anthropogenic processes that have resulted in increasing concentration of Sb in the environment, and also because of its impacts and possible adverse effects to living organisms. Several techniques have been used, to obtain reliable results for Sb, since Sb is present at low level concentration, requiring analytical instrumentation with low detection limits. The neutron activation analysis (NAA) technique has a high metrological level for the determination of several elements in different matrices. However, Sb determination in environmental and biological samples presents some analytical difficulties due to its low concentrations and gamma ray spectrum interferences. The objective of this research was to study on Sb determination in environmental reference materials by NAA. Ten environmental reference materials were selected and analyzed using long period irradiation at IEA-R1 research nuclear reactor. The induced gamma activities of ¹²²Sb and ¹²⁴Sb were measured. Relative errors of the results demonstrated that the accuracy depends mainly on Sb radioisotope measured, the decay time for counting and the sample composition.     

GammaLab: a suite of programs for k0-NAA and gamma-ray spectrum analysis

The GammaLab is a collection of computer codes, written in MATLAB, for performing calculations involved in k ₀ neutron activation analysis. The main features of the program include calibrations including energy-channel, energy-FWHM and energy-efficiency for different geometries, background subtraction, nuclide identification, spectral interference correction, elemental concentration and limit of detection determination. The data input is taken from two files one is the spectrum file stored in IAEA ASCII format and other is report file containing peak energy and peak area data. The information about sample, irradiation and counting conditions, background spectra are retrieved from QAQCData database. GammaLab takes nuclear data such as gamma lines, emission probabilities, half-lives, and k ₀ factors from NucData database. The sample results which contain elemental concentrations with uncertainties are stored in the QAQCData database. The program has been evaluated by analyzing several hundred spectra and results were found satisfactory.     

Decreasing the detection limits to ppq levels for high purity silicon analysis by instrumental neutron activation analysis with kilogram sampling weight

The amount of silicon sample used in instrumental neutron activation analysis (INAA) is generally less than twenty grams and the detection limits are in the range of ppb to ppt. The detection limits can be decreased further in several ways. Increasing neutron flux density, extending irradiation period and/or using more effective detector can improve the detection limits to some extent. Increasing sample weight, however, is a more feasible way to decrease the detection limits by a factor of hundreds with no new investment in existing irradiation/counting systems. In this work, two 8-inch high-purity silicon samples were analyzed by INAA to evaluate the validity and limitations of this concept in respect to neutron flux inhomogeneity, neutron shielding and -ray counting efficiency.     

Standardizing NAA of biological samples of varying size, shape and composition

Neutron activation allows the analysis of wet and dry biological tissues without sample preparation. To eliminate the need to prepare standards of each element to match each sample, we have standardized for a small number of typical sample types and irradiation and counting conditions. Then, for each sample analyzed, the concentration calculation includes corrections to the neutron flux and the counting efficiency, which depend on sample size and composition. The effects corrected include the neutron flux gradient in the irradiation site, the moderation of the neutrons with the hydrogen content of the sample and the variation of counting efficiency with sample volume. This revised version was published online in August 2006 with corrections to the Cover Date.     

Determination of noble metals by neutron-activation analysis

The scope and limitations of neutron-activation analysis in the field of the platinum metals are discussed. Special attention is given to interferences that occur in determination of noble metals in platinum metals and in natural samples. The problem of standards, carriers and chemical yield determination is emphasised. A recommendation is given of modern techniques for counting radionuclides formed by neutron activation of the platinum metals.     

Numerical Stability Problems in the K0-Standardization Method for the Case of Short Irradiation and Counting Times

The k ₀-standardization method of neutron activation analysis (NAA) is very sensitive to the irradiation and counting time during measurement of the induced radionuclide by -spectrometry on the HP Ge detector. If the irradiation and counting time of the sample and co-irradiated standard is relatively short or the decay constant small, the application of the standard equation in the software for the specific count rate may become numerically unstable and the program aborts. In this work, attention is focused on the direct influence of saturation and "measurement" factors on the specific count rate for simple decay and for more complex types calculated directly by exponential functions, and by an alternative form using a truncated Taylor's series expression.     

Evaluation of reactor pulsing activation analysis enhancement in reference materials

The enhancement factors possible by using reactor pulsing during neutron activation analysis have been shown to exceed 1.0 for half-lives shorter than 42 seconds. Studies published to date have applied the technique to pure elemental standards in order to evaluate the advantage. In addition, its use has been demonstrated for the analysis of several environmental samples. This paper describes experimental work performed in an effort to demonstrate the utilization of the technique on a wide range of real sample materials. The purpose of the investigation was to assess the value of the methodology to the neutron activation analysis program of our laboratory in support of university research. A series of sample matrices including reference materials, fossil fuels, geological specimen, ecologically important materials and animal and plant tissues have been subjected to pulsed neutron irradiation. Resulting gamma emissions were detected from samples after each irradiation. Representative spectral data are presented. Suitability of the technique for trace analysis are discussed.