Quantitative aspects of neutron activation analysis and isotope production with a small reactor

The use of “small” research reactors with applicable thermal neutron fluxes of ≤10^12.cm^−2.s⁻¹ in (instrumental) activation analysis based on γ-spectrometry, and in isotope production for radiotracer experiments is surveyed on the absis of the experience at ECN, Petten, The Netherlands and elsewhere. The aim is to provide a practical guideline for the application of “small” reactors in both fields. Reproducibility and knowledge of the physical parameters of irradiation and counting are essential and thus the first task of the radioanalyst. Emphasis is laid on the use of short-lived radionuclides. This implies the elimination of an additional source of bias in γ-spectrometry. Some suggestions are made on eventual projects of current interest.     

Kinetic aspects of the syntheses using short-lived radionuclides

“ACTIVA” is an activation analysis programme written for small computers (16 to 32 k-words) in FORTRAN-IV. Input-mode for operating commands is interactive, guided with self-explenatory questions. This enables the evaluation of gamma-spectra which could be registered under 4 different conditons (flux, geometry, etc.) with two different counting systems existing in Atominstitute. In each case another data-library with different calibration factors will be chosen and used automaticly. Programme “ACTIVA” is originally designed for gamma-spectra registered with “Loss-Free-Counting” (LFC) electronic with 2×2048 channels, but can be modified for 1024 or 4096 channels easily. Two different multichannel analysers (MCA) can be chosen for data-input: ORTEC-6240 MCA, or NOVALFC (Loss-Free-Counting). The correct energy calibration constants will also be chosen automaticly. The programme has a modular constraction and combined (linked) with overlay technique.     

Analyse par activation non destructive: Contribution a l'etude des conditions d'analyses exactes

In non destructive activation analysis, either relative measurements or parametric counting techniques are used. However, in so complex media as biological or geological samples, where a lot of radionuclides are produced, an accurate determination of an element, must take into account, the “background shape and height effect” due to the other radionuclides. To achieve accuracy in such determinations, a new method is developed.     

Experimental comparison of multi-channel analyzer. Dead-time corrections for short-lived radionuclides

The accuracy of the live-time circuit of a 400-channel analyzer was studied in detail, and was found to be unsatisfactory even for long-lived radionuclides. It was found that automatic live-time correction with the multi-channel analyzer gave rise to increasing positive errors with increasing count rate; this overall positive error was composed of a positive error due to the slowness of the electronic circuitry, and a smaller negative error due to the finite pulse-width. Adequate correction could be performed by feeding the information from the dead-time output of the multi-channel analyzer to an external live-time circuit with variable oscillator frequency and pulse-width. Four methods for dead-time correction were compared experimentally in the case of short-lived radionuclides (T as low as 7 sec): the method of Bartošek et al., the method of Schonfeld, the use of a sufficiently short counting time as compared to the half-life, and the live-time mode of counting without additional correction. These four methods were applied to the determination of oxygen and silicon in rocks by 14 MeV neutron activation analysis. Results are given for USGS standard rock G-2. Research associate of the I. I. K. W.     

Direct counting of soil wafers: An improved total alpha/beta screening analysis

Although potentially very useful as a screening tool, currently-applied “gross” alpha/beta analyses are often considered unreliable by the environmental monitoring community. We describe here an alternative approach based on direct counting of pressed soil “wafers” to estimate total alpha/beta activities. The system was calibrated using a series of natural soils and sediment standards with total α/β activities estimated by use of a combination of available certified values, equilibrium assumptions, and our own measurements. A set of 10 such standards that span a wide range of activities were prepared by thoroughly mixing several grams of selected NIST and IAEA natural matrix standards together with reagent grade cellulose in a 4∶1 sample-to-binder ratio and pressing in a 40-mm stainles steel die. The resulting wafers, assumed to be at infinite thickness for expected radionuclides, were counted in a gas flow proportional counter set for simultaneous α/β counting. Both the alpha and beta count rates increased in a linear, systematic manner with increasing total estimated activities. This technique should prove to be an inexpensive, simple, and waste-free approach for screening total radioactivity in soil samples.     

A software counting loss correction method for neutron activation analysis with short-lived radionuclides

A method has been developed for the correction of counting losses in NAA for the case of a mixture of short-lived radionuclides. It is applicable to systems with Ge detectors and Wilkinson or successive approximation ADC's and will correct losses from pulse pileup and ADC dead time up to 90%. The losses are modeled as a constant plus time-dependent terms expressed as a fourth order polynomial function of the count rates of the short-lived radionuclides. The correction factors are calculated iteratively using the peak areas of the short-lived radionuclides in the spectrum and the average losses as given by the difference between the live time and true time clocks of the MCA. To calibrate the system a measurement is performed for each short-lived nuclide. In a test where the dead time varied from 70% at the start of the measurement to 13% at the end, the measured activities were corrected with an accuracy of 1%.     

Chemical speciation code CHEMSPEC and its applications

The adsorption and migration behavior of a radionuclide in geological media heavily depends on its chemical forms in a given chemical environment. In order to predict the temporal and spatial distribution of radionuclides around a disposal site when its canister is damaged, it is necessary to develop coupled chemical speciation-solute transport models and relevant software. For that reason, we wrote a new chemical speciation program CHEMSPEC. In this paper, the principles and structure of CHEMSPEC are briefly described, and the strategy and algorithms that were used in this code are interpreted in some detail, such as the measures adopted to prevent divergence in iteratively solving the mass balance equations, the “predictor-corrector” algorithm for calculation of the number and quantities of solid species formed, and the alternate use of “freezing” and “defreezing” oxidation states in handling of co-existent redox and precipitation equilibria. Four examples are given to illustrate CHEMSPEC’s features and capabilities.     

Identification of unknown nuclear reaction products using gas phase separation and chemical pattern analysis

A method for the fast separation of short-lived nuclides in the gas phase is described. The attribution of new γ-lines to a certain element is possible by the variation of the chemical and physical separation parameters and the determination of the “yield” of a line, compared with the “yields” of well known nuclides.     

Development of the <Emphasis Type="Italic">k</Emphasis><Subscript>0</Subscript>-based cyclic neutron activation analysis for short-lived radionuclides

The k ₀-based cyclic neutron activation analysis (k ₀-CNAA) technique has been studied to explore the applicability at the Portuguese research reactor (RPI). In particular, for the determination of elements which form short-lived radionuclides, particularly fluorine (²⁰F, 11.16 s half-life) and selenium (^77mSe, 17.36 s half-life) in polymer, biological and environmental samples. The detection limits obtained for F and Se were about 50 and 0.01 mg kg⁻¹, respectively, in the investigated materials. The timing parameters for the procedure were 10 to 20 s for irradiation, 5 s decay, 10 to 20 s counting, 5 s waiting and performed with eight cycles. The k ₀-IAEA program was modified to use millisecond time resolution for irradiation, decay and counting times as needed for interpreting k ₀-CNAA data in terms of concentration, accuracy and detection limit. The quality control of the procedure was performed by preparing a standard solution containing fluorine with different contents as well as using the certified reference materials containing selenium from which the bias between the results and the certified values were within 15% for most elements at the investigated content ranges. The analytical results for several other elements producing short-lived or detectable radionuclides, e.g., Al, Ca, Cl, Cu, Dy, I, Mg, Mn, Ti, and V were also obtained by the k ₀-CNAA procedure with accuracy within 12%.     

A simple program in “basic” language for analysis of gamma-spectra using an on-line minicomputer

A program in “INSTRUMENT BASIC” language is proposed for analysis of gamma-ray spectra obtained with Ge(Li) detectors and accumulated in multichannel analysers on-line with minicomputers. The program locates the peaks, evaluates the corresponding energy values, the net peak areas and the standard deviations on the areas.     

Fast neutron activation analysis using short-lived radionuclides

Fast neutron activation analysis experiments were performed to investigate the analytical possibilities and prospective utilization of short-lived activation products. A rapid pneumatic transfer system for use with neutron generators has been installed and applied for detecting radionuclides with a half-life from 300 ms to 20 s. The transport time for samples of total mass of 1–4 g is between 130 and 160 ms for pressurized air of 0.1–0.4 MPa. The reproducibility of transport times is less than 2%. The employed method of correcting time-dependent counting losses is based on the virtual pulse generator principle. The measuring equipment consists of CAMAC modules and a special gating circuit. Typical time distributions of counting losses are presented. The same 14 elements were studied by the conventional activation method (single irradiation and single counting) by both a typical pneumatic transport system (run time 3 s) and the fast pneumatic transport facility. Furthermore, the influence of the cyclic activation technique on the elemental sensitivities was investigated.     

Determination of Al,Ca, V and Mn by INAA: Application to the Reference Material IAEA-395 “Urban Dust”

Instrumental NAA based on short-lived radionuclides implies high initial total count rates which change appreciably over the counting period. This in turn necessitates corrections for three negative biases: losses due to differences in counting time between samples and standards; pile-up losses, and (residual) influence of dead-time. The procedure is demonstrated for the determination of Al, Ca, V and Mn in the IAEA Reference Material 395 Urban Dust. The obtained data are in good agreement with the reference values for this material. By limiting the total relative dead-time to 25%, statistical uncertainties are below 5%.     

Calibration of activity readings from radiopharmaceuticals with impurities

Accurately determining the amount of a radionuclide actually administered to a patient is an important aspect of quality control in nuclear medicine. In this study, in order to accurately assess the “apparent” radioactivities of radionuclides with impurities by a dose calibrator, two methods, (1) curve fitting, and (2) relative sensitivities calculation, have been employed to determine the parameter, M (relative response). From the comparisons between the measurement and re-calculated radioactivity using the M values, each method was found to have its own advantage and disadvantage, depending upon the fraction ratio of the impurity as well as the energy level of the impurity’s photons. This study might be helpful for improving the assessment of radiopharmaceuticals’ “true” activity and its “apparent” activity measured by a dose calibrator.     

Methodology for the U.S. Food and Drug Administration's radionuclides in foods program

The U.S. Food and Drug Administration (FDA) is responsible for the wholesomeness of the nation's food supply. The FDA modified its food monitoring program in January, 1973, to include radioactive isotopes. The methodology used to perform, analyses on these food products are taken from the standerd setting societies such as the AOAC International, American Society for Testing Materials and American Public Health Association Standard Methods. In addition, methods not tested by these societies are taken from the literature or from Department of Energy manuals such as the Health and Safety Laboratory and also from Environmental Protection Agency, Public Health Service, and Food and Agricultural Organization manuals. These include the methods for long-lived radionuclides such as tritium, strontium-90, cesium-137 and plutonium. Also, the short-lived radionuclides such as iodine-131, radiocesium, radiocerium and radioruthenium. In addition, they include the natural occurring radionuclides such as radium and uranium isotopes. The activity concentrations of gamma-emitters such as radiocesium, iodine-131 and radioruthenium are determined by gamma-ray spectrometry. This is done using intrinsic germanium detectors with the appropriate hardware and software. The alpha and “pure” beta-emitters are determined by various radiochemical methods and techniques. The radiochemical methodology and equipment used in analyzing these radionuclides are described and discussed. Also, the methodology and equipment for the gamma-emitters are described in more detail in this paper. In addition, the limits of detection for the methods used will be discussed.     

Actual state of high-rate digital gamma-spectrometry

Two commercially available digital filters with selectable, fixed time constants and triangular pulse response are discussed to outline their potential advantages over traditional analog filters with semi-Gaussian pulse shape. A solution for the “resolution or throughput rate” dilemma is offered by the preloaded digital filter fulfilling the postulate for the ideal adaptive filter with optimum resolution at any counting rate. Throughput rates of >100 kc/s are demonstrated for the preloded digital filter at resolutions superior to those of fixed shaping time filters.     

Migration of85Sr and137Cs in vertical soil profiles

The vertical distribution of⁸⁵Sr and¹³⁷Cs in undisturbed single-contaminated agricultural soils have been studied during their irrigation with wet atmospheric precipitation in dependence on time under laboratory conditions for about one year. The soil samples were collected from several localities in the environment of nuclear power plants at Dukovany and Jaslovské Bohunice using a special auger. The samples were placed into polyethylene columns of 9 cm in diameter and 20 cm in height. The activity of radionuclides in soil profiles after their separation into single layers were counted by Ge(Li) semiconductor gamma-spectrometry. Based on the exponential depth distribution of radionuclides, the values of their migration parameters as relaxation depth, migration rate and retardation factor were calculated. The influence of the permanent grass cover and of the applied zeolite on the migration parameters of these radionuclides was also investigated. Presented at the Conference “Nukleonika '98”, Prague, Czech Republic, 9–10 September 1998, dedicated to late Professor František Běhounek in honour of his 100th birthday.     

Critical points on vapor-liquid stratification curves in inhomogeneous systems

A historical information about the introduction of one of the main concepts in the theory of condensed phases, critical point, is given. The initial term, “absolute boiling temperature,” introduced by D.I. Mendeleev was formulated on the basis of deeper views on the nature of critical phenomena than later studies by T. Andrews, who suggested the term “critical temperature,” which became well established with time. Most interesting estimation of the studies by Andrews was given by D.I. Mendeleev. The concept of critical temperature and the investigations of D.I. Mendeleev were discussed.     

The transfer of natural (226Ra,?232Th, 40K) and artificial (137Cs, 90Sr) radionuclides from soil to the wood of a Scots pine (Pinus sylvestris L.)

On the Stabatishke site near to Ignalina Nuclear Power Plant a near surface repository for low and intermediate-level short-lived radioactive waste is being constructed to store the waste which was produced during the decommissioning of the Ignalina Nuclear Power Plant. A possible spread of radionuclides from the near surface repository and the radiation level of expression are one at the most important aspects while evaluating the safety of the repository. The article examines the specific activity of artificial (¹³⁷Cs, ⁹⁰Sr) and natural (²²⁶Ra, ²³²Th, ⁴⁰K) radionuclides in the soil of Stabatishke site of Ignalina NPP in pinewood; the spread of these radionuclides is determined in the system “soil-tree”. The change of long term soil pollution with artificial radionuclides was estimated. This is a background soil pollution which had been there before the exploitation of the near surface waste repository. The transfer factors of natural (²²⁶Ra, ²³²Th, ⁴⁰K) and artificial (¹³⁷Cs, ⁹⁰Sr) radionuclides from the 0-to-20-cm soil layer to different annual pinewood rings were measured. After estimation of the position of pine roots in accordance to the soil vertical and the annual change of the plant biomass, the transfer factor of ¹³⁷Cs movement to different annual pinewood rings from the separate 0 to 20-cm soil layers was determined.     

Normalized Lempel-Ziv complexity and its application in bio-sequence analysis

In this article, we propose a new method to measure DNA similarity based on a normalized Lempel-Ziv complexity scheme. The new method can weaken the effect of sequence length on complexity measurement and save computation time. Firstly, a DNA sequence is transformed into three (0,1)-sequences based on a scheme, which considers “A” and “non-A” , “G” and “non-G”, “C” and “non-C” bases respectively. Then, the normalized Lempel-Ziv complexity of the three (0,1)-sequences constitute a 3D vector. Finally, by the 3D vector, one may characterize DNA sequences and compute similarity matrix for them. The examination of similarities of two sets of DNA sequences illustrates the utility of the method in local and global similarity analysis.