A critical evaluation of short-lived and long-lived neutron activation products for trace element determinations

The application of short-lived nuclides in routine instrumental neutron activation analysis can reduce total experimental time per sample. The experimental sensitivities of short- and long-lived thermal neutron activation products of 32 elements are compared. The advantages of using short-lived nuclides are evaluated by comparing the precision, accuracy, and detection limits, using both short- and long-lived nuclides, for elemental determinations in biological, environmental and geological standard reference materials.     

The correlations among various elements in neutron activation analysis — The evaluation of R-matrix and κ-matrix

The production rates (numbers of atoms per gram of the respective elements per second) of 40 radioactive nuclides of 34 elements by neutron capture reactions in a reactor were determined from about 130 photopeaks of the -ray spectra. The ratios of these production rates were called R-matrix elements. These production rates and the respective thermal neutron capture cross sections were used to calculate the respective apparent neutron fluxes at the position of irradiation and the -matrix elements which were the ratios of these apparent neutron fluxes. These matrix elements express clearly the correlations among various elements and thus may be used in the mono-standard or small-number-standards method in neutron activation analysis.     

Reactor neutron activation analysis by using multi-elemental comparators: Problems of nuclear constants of128I,175Yb and several other nuclides

A simple method has been developed for evaluating the neutron spectrum and the temperature by using U, Sb, Cr, Co and Lu as monitors and successfully applied to the routine analysis. For most of nuclides, amounts determined by the method showed reasonable agreements with those added. However, there have been found several nuclides which gave erroneous results beyond the permissible limits. In the case of¹²⁸I, the reason for the deviation was found to lie on the normalization factor of -ray abundances that are in common use. This was confirmed by using I₂ doped polyacethylene which is a material highly resistant to ionizing radiations.⁴⁶Sc,¹⁷⁵Yb and several other rare earth nuclides are discussed as well.     

Elemental analysis in bed sediment samples of Karnafuli estuarine zone in the Bay of Bengal by instrumental neutron activation analysis

The concentration of rare earths and other elements have been determined in the bed sediment samples of Karnafuli estuarine zone in the Bay of Bengal by instrumental neutron activation analysis (INAA). The samples and the standards soil-5, soil-7, coal fly ash and pond sediment were prepared and simultaneously irradiated for short and long time at the TRIGA Mark-II research reactor facility of Atomic Energy Research Establishment, Savar, Dhaka. The maximum themal neutron flux was of the order of 10¹³ n·cm^–2·s^–1. After irradiation the radioactivity of the product nuclides was measured by using a high resolution high purity germanium detector system. Analysis of -ray spectra and quantitative analysis of the elemental concentration were done via the software GANAAS, it has been possible to determine the concentration level of 27 elements including the rare earths La, Ce, Sm, Eu, Tb, Dy and Yb and uranium and thorium.     

Neutron activation analysis without multielement standards

A physical approach is described for instrumental multielement activation analysis with whole neutron spectrum (without Cd-cover) using the monostandard (single comparator) method. To test the capabiliteries of this method, 15 samples representing different Egyptian granite rocks were analyzed. As many as 21 trace elements beside Fe, K and Na were determined. Calculation of the experimental data has been done using the Gamma-Monostandard Analysis program with the Commodore Computer available at the Institute of Radiochemistry at Garching near München. The accuracy of the method for nondestructive multielement analysis agrees within 3% with the relative method using multielement standards.     

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.     

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.     

Information Obtained by Three Different Methods of U and Th Determination in Sediment and Algae Samples from the Romanian Sector of the Danube River and the Black Sea Coast

The concentration distributions of U and Th nuclides in some sediment and algae samples from the Romanian sector of the Danube river and the Black Sea coast are presented. Data are obtained by neutron-induced fission activation analysis, epithermal instrumental neutron activation analysis and radiochemical separation using tracers followed by -spectrometry counting of stainless steel discs after electrodeposition. The analysing time, the working steps, the necessary equipment, the information and quality of the obtained results are discussed.     

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.     

Epithermal neutron activation analysis using the monostandard method

A method is described for epithermal neutron activation analysis of 17 elements in granite rock samples using a single standard. Gold has been used as a single comparator due to its relatively high resonance integral value (I₀=400 barn). In addition, it is preferable to Co in order to obtain a large epithermal activation in a short irradiation. The method of calculation is simple and rapid and can be done using a small calculator. Epithermal activation is able to overcome the difficulty arising from changing irradiation position as well as increasing the number of determinable elements by eliminating the interference from undesired isotopes which have relatively high thermal cross section values (₀), when reactor neutron flux is used. The coupling of epithermal activation with the monostandard method has the advantage of using a small Cd-cover which overcomes most of the difficulties arising in the relative method with large volume cadmium filters.     

Recent developments in HYPERMET PC

HYPERMET PC is a user-friendly -ray spectrum analysis software package developed at Budapest, mainly for the purpose of prompt- neutron activation analysis (PGAA). The peak fitting algorithm is an improved version of the well-known HYPERMET code, and contains a partial peak-parameter calibration to describe peak shapes more accurately in the wide energy range typical for prompt- spectra. A nuclide identification routine has also been developed using a new PGAA library, shown in a parallel paper. The new module for quantitative PGAA includes all the features necessary to obtain concentration values for elements.     

Interference by neutron induced second order nuclear reaction in activation analysis of platinum group elements after a nickel sulphide fire assay preconcentration

In determining the trace platinum group elements and gold in rocks and ores by the neutron activation analysis after a nickel sulphide fire assay preconcentration, there are interferences due to nuclides produced from second order nuclear reactions. This paper presents the degree of interference calculated over the ranges of long irradiation times and of reactor neutron flux from 1·10¹³ to 1·10¹⁵ n·cm^–2·s^–1. According to the results of these calculations, every one of the second order interfering reactions on the PGE+Au, except the¹⁹⁷Au(n, )¹⁹⁸Au(n, )¹⁹⁹Au reaction, can be neglected under the long irradiation time or high reactor neutron flux. Special attention is given to the interference from gold in the determining platinum.     

A new approach to single-comparator instrumental neutron activation analysis

A new parametric approach to single-comparator instrumental neutron activation analysis (INAA) at the University of Missouri Research Reactor (MURR) was investigated. A detailed MCNP steady-state model of the MURR core was developed using the latest neutron data libraries to compute the continuous-energy neutron flux distribution. Intrinsic reaction rates were predicted by coupling the computed local flux distribution to the isotopic (n, γ) excitation functions for a range of elements present in standard reference materials (SRM). Using the predicted (n, γ) reaction-rates, the concentrations for the various elements were determined. The method worked well for all nuclides tested, including those with cross sections that are not proportional to 1/v such as Lu and Eu with agreements for most elements within 5% of the reference value.     

Comparison Method for Neutron Activation Analysis with γ-γ Matrix

A comparison method, utilizing neutron activation analysis followed by multidimensional spectrum analysis was proven to provide accurate quantification of the multi-element samples. In this study, 23 elements were detected simultaneously in a sample containing standard elements for neutron activation analysis. The method presented here can be applied for about 50 elements.     

Review of neutron activation analysis in the standardization and study of reference materials, including its application to radionuclide reference materials

Summary Neutron activation analysis (NAA) plays a very important role in the certification of reference materials (RMs) and their characterization, including homogeneity testing. The features of the method are briefly reviewed, particularly aspects relating to its completely independent nuclear basis, its virtual freedom from blank problems, and its capacity for self-verification. This last aspect, arising from the essentially isotopic character of NAA, can be exploited by using different nuclear reactions and induced nuclides, and the possibility of employing two modes, one instrumental (nondestructive), the other radiochemical (destructive). This enables the derivation of essentially independent analytical information and the unique capacity of NAA for self-validation. The application of NAA to quantify natural or man-made radionuclides such as uranium, thorium, ²³⁷Np, ¹²⁹I and ²³⁰Th is discussed, including its advantages over conventional radiometric methods, and its usefulness in providing independent data for nuclides where other confirmatory analyses are impossible, or are only recently becoming available through newer atom counting techniques. Certain additional, prospective uses of NAA in the study of RMs and potential RMs are mentioned, including transmutation reactions, creation of endogenously radiolabelled matrices for production and study of RMs (such as dissolution and leaching tests, use as incorporated radiotracers for chemical recovery correction), and the possibility of molecular activation analysis for speciation.     

Monte Carlo source simulation technique for solution of interference reactions in INAA experiments: a preliminary report

A new method using Monte Carlo source simulation of interference reactions in neutron activation analysis experiments has been developed. The neutron spectrum at the sample location has been simulated using the Monte Carlo code MCNP and the contributions of different elements to produce a specified gamma line have been determined. The produced response matrix has been used to measure peak areas and the sample masses of the elements of interest. A number of benchmark experiments have been performed and the calculated results verified against known values. The good agreement obtained between the calculated and known values suggests that this technique may be useful for the elimination of interference reactions in neutron activation analysis.     

Chemical separation procedure for the nuclide analysis of a tantalum target irradiated for 500 days with 800 MeV protons

A rapid radiochemical separation procedure has been developed for the determination of long-lived and stable nuclides produced by spallation and activation in a tantalum target irradiated for 500 days with 800 MeV protons. In this procedure the matrix element tantalum and simultaneously the¹⁸²Ta activity, built-up by activation of the matrix with themalized spallation neutrons is removed from many elements. About 50 mg of the sample is dissolved in a mixture of concentrated nitric and hydrofluoric acid. After dilution tantalum is extracted with a solution of 0.2M tetrahexylammonium bromide in methyl isobutyl ketone (MIBK). The residual amount of tantalum and the remaining¹⁸²Ta activity are 0.0003% and the recoveries of 27 investigated elements are in the range of 96.0–99.9%. A further 22 elements are quantitatively separated according to their chemical behavior. In the final aqueous fraction the separated long-lived and stable nuclides of 49 elements can be measured with high sensitivity by -ray spectrometry and mass spectrometry (ICP-MS).     

Neutron scattering by hydrogen in cold neutron prompt gamma-activation analysis

The effects of neutron scattering by hydrogen within targets for cold neutron prompt -ray activation analysis (CNPGAA) have been characterized. For most targets studied, the probability for neutron absorption, and hence CNPGAA sensitivities (counts·s^–1·mg^–1), decrease with increasing H content and with target thickness. Comparisons with results from thermal neutron PGAA indicate that the effects of cold neutron scattering differ from those of thermal neutron scattering. CNPGAA sensitivities for l/v nuclides show similar sensitivity decreases, while Sm sensitivities show smaller decreases.     

Determination of rare-earth elements in rock samples by neutron activation analysis with a lithium-drifted germanium detector after chemical group-separation

A lithium-drifted germanium detector combined with chemical group-separation has been utilized for the determination of rare-earth elements (La, Ce, Nd, Sm, Eu, Gd, Tb, Tm, Yb and Lu) in rock samples by neutron activation. This procedure has the advantage of a low background level which cannot be attained in the non-destructive method. The combination of the Ge(Li) detector and chemical group-separation also offers a distinct simplification in the correction of contributions from other nuclides. For optimum utility of a Ge(Li) detector in neutron activation analysis, chemical group-separations are recommended.