The influence of sample properties and sample geometry on the accuracy of gamma-ray spectrometric analyses

Nuclear isomers of half-lives above one second have been excited from the ground state of stable nuclides via inelastic γ-ray scattering by using bremsstrahlung of a 4 MeV, 22 μA linear electron accelerator. This method is potentially useful for a number of elements in elemental analysis by virtue of its high specificity and, in some cases good sensitivity. As there is no need for special sample preparation, this kind of activation may be preferable in some applications. Detection sensitivities have been determined for 15 elements, and possibilities in routine chemical analysis are discussed.     

Seasonal variations of radionuclide concentrations in pine needles

Seasonal variations of radionuclide concentration in pine needles (Pinus Thunbergii) were examined. The seasonal variations were classified roughly into two types, one represented by the periodical variation of¹³⁷Cs concentration and the other represented by a linear decrease of¹⁰³Ru concentration when plotted on a semi-log scale. Weathering half-lives for the latter type of nuclides were estimated and a fairly good consistency in the half-lives for different nuclides was observed irrelevant to their radioactive half-lives.     

Quantitative activation analysis of the target assemblies of a medical linear accelerator

Radioactive nuclides with relatively long half-lives in the target assemblies of medical accelerators were investigated. The samples were the target assembly of a 10 MV linear accelerator, a 20 MV microtron and screws of a cyclotron. Gamma-spectroscopy was performed with a high-purity germanium (HPGe) detector. Detected nuclides were ⁵¹Cr, ⁵⁴Mn, ⁵⁹Fe, ⁵⁷Co, ⁵⁸Co, ⁶⁰Co, ⁶⁵Zn, ^108mAg, and ^110mAg. As the half-lives of some generated nuclides are relatively long, it is difficult to adapt to decay-in-storage.     

Studies of short-lived fission products by means of the multistage solvent extraction system SISAK

The multistage solvent extraction system SISAK is described. The system is used for online studies of nuclides with half-lives down to 1 s. Some of the chemical separation procedures are presented, and a survey is given on the results obtained so far. The possiblity to gain access to nuclides with even shorter half-lives is also discussed.     

Progress in Activation Analysis at the Atomic Institute Vienna

Fields in which progress has been achieved at the Atomic Institute Vienna are discussed briefly. The use of short and medium lived nuclides for activation analysis (AA). Construction of out-core parts of a fast transfer system. Combined sample catcher sample-changer for AA allowing cyclic and pseudocyclic AA. A system for discontinuous or continuous irradiation of liquid samples. Counting with an anticompton shield and quantitative correction of random coincidences. Screening analyses with the fast irradiation and measurement system. Improved peak-evaluation of gamma-spectra. Epithermal AA by a neutron converter. Following short-lived nuclide measurement, automatic sample transfer into a well-type detector enabling sensitive counting of nuclides with short half-lives. Use of large samples to increase the detection limits of ng to pg at activation with moderate neutron flux. Flux determination by liquid scintillation counting.     

Use of chromatographic pre-concentration for routine uranium bioassay analysis by ICP-MS

Routine monitoring of urine is an effective way to detect occupational intake of radioactive material. Historically, determinations of uranium isotopic ratios have been performed by radiochemical separation followed by alpha spectrometry. With recent advancements in technology, inductively coupled plasma-mass spectrometry (ICP-MS) has become widely available for the determination of trace metals as well as radioactive nuclides with long half-lives, such as ²³⁸U in urine. Furthermore, ICP-MS measurements of ²³⁸U do not require radiochemical separation since the number of atoms in the sample is determined instead of the number of alpha particles emitted. However, this method does not provide good sensitivity for the determination of ²³⁵U due to its shorter half-life. An improved procedure using pre-concentration of uranium and determination by ICP-MS decreases the detection limit by a factor of ten or greater with only slight increase in total analysis time. The method also has the capability of accurately determining the isotopic ratio of the sample, which is very important in cases where enriched or depleted uranium is involved.     

"Sand bar" of actinoid and neighboring elements in a chart of nuclides

Inspection of a chart of nuclides reveals a "sand bar" of actinoid and neighboring elements when a suitable half-life level is chosen. A bay of alpha-instability lying between the nuclides of neutron magic number 126 and the beta-stability line in the actinoid group is a characteristic feature in this area. Calculation shows that fairly good agreement is obtained between the measured half-lives and those derived theoretically.     

Instrumental activation analysis of coal and fly ash with thermal and epithermal neutrons and short-lived nuclides

Instrumental neutron activation analysis is applied to the determination of about 25 elements in coals and fly ash by means of nuclides with half-lives of less than 48 h ; thermal and epithermal irradiations are used. The results indicate that epithermal activation is preferable for twelve of the elements (Ga, As, Br, Sr, In, Cs, Ba, La, Sm, Ho, W and U). Data for SRM 1632 (coal) and SRM 1633 (fly ash) compare favorably with the results obtained by other investigators.     

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.     

Characteristics of formvar films used to prevent alpha-detector contamination

Alpha spectrometry is an extremely useful and sensitive for detection of alpha-emitting nuclides. Contamination of the silicon detectors for low-level alpha spectrometry by recoil nuclides is a serious problem in the measurement of alpha emitters decaying to daughter nuclides with short half-lives. This unwanted contamination leads to decreased measurement sensitivity causing a degradation of the limit of detection. The simplest method to prevent this radioactive contamination of detector is to use a catcher film between the alpha source and the detector. In this work we describe the obtaining of the thin formvar films as stopper foils for recoil nuclei and we investigated the influence of these films on alpha spectrometry parameters, as energy shift (~30 keV) and resolution (~7%). No significant deterioration of the alpha spectrometry parameters was observed when using thin formvar films. Using the ASTAR web databases, which calculate stopping powers for alpha particles, the thickness of formvar films was estimated to be about 5.355 × 10⁻⁵ g/cm². The measurements were performed with an ORTEC SOLOIST alpha spectrometer with PIPS detector.     

Spontaneous 238U fission half-life measurements based on fission-track techniques

In the last recommendation of the International Union of Pure and Applied Chemistry (I.U.P.A.C.) on spontaneous fission half-lives for ground-state nuclides, a number of measurements of ²³⁸U based on fission-track techniques were discarded. The arguments given by the authors are not clear. In this work a more detailed discussion of these determinations is given, considering the possible systematical errors inherent in fission-track approaches.     

Determination of 34 elements in Chinese geochemical standard reference materials by instrumental neutron activation analysis

Thirty four elements (Al, As, Ba, Br, Ca, Ce, Co, Cr, Cs, Dy, Eu, Fe, Gd, Hf, Ho, K, La, Lu, Mg, Mn, Na, Nd, Rb, Sb, Sc, Sm, Ta, Tb, Th, Ti, U, V, W, Yb) were determined by instrumental neutron activation analysis in the second set of Chinese geochemical standard reference materials (sediments from GSD-9 to GSD-12, soils from GSS-1 to GSS-8, rocks from GSR-1 to GSR-6) using both thermal and epithermal irradiations. Irradiation schemes designed to utilise short, medium and long-lived nuclides were employed in order to analyse major, minor and trace elements with different half-lives. The gamma-ray spectra were measured by Ge(Li) and HP(Ge) detectors. Relevant nuclear data and possible interferences are listed, and analytical results are presented and discussed.     

Nuclide analysis of a tantalum target irradiated with high-energy protons

First results of γ-spectrometric measurements of radionuclides produced in a tantalum target irradiated for 500 days with 800 MeV protons are presented. The activities of the γ-ray-emitting nuclides measured after a cooling period of 2–4 years differ by more than four orders of magnitude. Within this cooling period about 95% of the activity of the target is determined by¹⁷²Lu,¹⁷³Lu,¹⁷⁴Lu,¹⁷²Hf (daughter nuclide of¹⁷²Lu) and¹⁸²Ta nuclides. These highly active nuclides, together with some other medium-active nuclides, were measured with good precision by γ-ray spectrometry directly in the sample solution. Weakly active nuclides could not be measured in this way because of the high Compton background in the γ-ray spectrum. For the sensitive measurement of many other nuclides present in weaker activities a simple chemical separation procedure was developed to separate Lu, Hf and Ta. With the separation of these elements and simultaneously of the high-active nuclides, the Compton background in the γ-ray spectra could be drastically reduced and many weakly active nuclides additionally measured.     

The half-lives of 90mY and 97Ru

In an attempt to improve the accuracy of neutron activation analysis, gamma-ray spectrometry and least-squares methods developed for other nuclides have been applied to redetermine the decay constants of ^90mY and ⁹⁷Ru. Several irradiated samples of each pure element were counted continually through several half-lives, acquiring up to 100 spectra with good statistics. Photopeaks from each nuclide were evaluated with a region of interest integration routine, and each data point corrected for rate-related losses before fitting to an exponential function by a nonlinear least-squares procedure. The half-lives found are 3.204 ± 0.008 h for ^90mY and 2.836 ± 0.014 days for ⁹⁷Ru, where the uncertainty is an estimate of the 95 % confidence level. Although (by Chi squared criteria) the fits to the decay curves were very good and the uncertainty of the resulting half-lives an order of magnitude smaller than the previously published uncertainty, care is necessary before assigning a best value with a totally defensible uncertainty to the overall data set.     

Cascade ultrafiltering of 210Pb and 210Po in freshwater using a tangential flow filtering system</p> </p>

Summary A rapid method was developed using ultrafilters with a tangential flow filtering system for molecular size separation of naturally occurring ²¹⁰Pb and ²¹⁰Po in a freshwater sample. Generally, ultrafiltering of a large volume water sample for measuring the nuclides was too time consuming and not practical. The tangential flow filtering system made the filtering time short enough to adapt for in-situ ultrafiltering the large volume sample. In this method, a 20 liter water sample was at first passed through the 0.45mm pore size membrane filter immediately after sample collection to obtain suspended particle matter [>0.45mm particulate fraction (PRT)]. Two ultrafilters (Millipore Pellicon 2^ò) were used sequentially. The nuclides in the filtrate were separated into three fractions: high molecular mass (100 kDa-0.45mm; HMM), low molecular mass (10 k-100 kDa; LMM) and ionic (<10 kDa; INC) fractions. It took 80 minutes to process the sample after collection. The cut-off molecular size of each ultrafilter was confirmed by size exclusion chromatographs (SEC) of the LMN and the HMM fractions. Adsorption of the nuclides and organic compounds in the sample onto the ultrafilters was negligibly small. Good reproducibility of the nuclide concentrations in each fraction was confirmed by repeated experiments. The method was successfully applied to obtaine the molecular size distributions of ²¹⁰Pb and ²¹⁰Po in an oligotrophic lake, Lake Towada located in the northern area of Japan.</p> </p>     

Quantitative portable gamma-spectroscopy sample analysis for non-standard sample geometries

Utilizing a portable spectroscopy system, a quantitative method for analysis of samples containing a mixture of fission and activation products in nonstandard geometries was developed. This method was not developed to replace other methods such as Monte Carlo or Discrete Ordinates but rather to offer an alternative rapid solution. The method can be used with various sample and shielding configurations where analysis on a laboratory based gamma-spectroscopy system is impractical. The portalle gamma-spectroscopy method involves calibration of the detector and modeling of the sample and shielding to identify and quantify the radionuclides present in the sample. The method utilizes the intrinsic efficiency of the detector and the unattenuated gamma fluence rate at the detector surface per unit activity from the sample to calculate the nuclide activity and Minimum Detectable Activity (MDA). For a complex geometry, a computer code written for shielding applications (MICROSHIELD) is utilized to determine the unattenuated gamma fluence rate per unit activity at the detector surface. Lastly, the method is only applicable to nuclides which emit gamma-rays and cannot be used for pure beta or alpha emitters. In addition, if sample self absorption and shielding is significant, the attenuation will result in high MDA's for nuclides which solely emit low energy gamma-rays. The following presents the analysis technique and presents verification results using actual experimental data, rather than comparisons to other approximations such as Monte Carlo techniques, to demonstrate the accuracy of the method given a known geometry and source term.     

Further results in search for transuranium elements in effluents discharged to air from nuclear power plants

In this work we present data on transuranium nuclides ²³⁸Pu, ^239,240Pu, ²⁴¹Am, ²⁴²Cm and ²⁴⁴Cm in effluents discharged to air (activity concentrations and annually discharged activities of individual radionuclides) from 7 stacks in 2004–2009. In the effluents discharged to air from one stack low activities of transuranium nuclides were observed throughout the studied period. Transuranium nuclides had been discharged to air from this stack also in previous years since 1996 when defect in the cladding of a fuel element and consequent contamination of the primary circuit occurred. In the effluents discharged to air from another stack transuranium nuclides were observed only in some monitoring periods of studied years. We could not prove the presence of transuranium nuclides in the effluents of the other stacks up to 2006. The transuranium nuclides in discharged effluents were registered in the second half-year of 2006. In 2007–2008 especially low activities of ²⁴¹Am were found in these effluents.     

The simultaneous determination of 235U and 239Pu using delayed neutron activation analysis

Delayed neutron activation analysis (DNAA) remains one of the most sensitive methods of nondestructively determining fissile materials in a variety of sample matrices, provided that the samples contain only a single fissile component. This has historically been the limiting factor in many applications of DNAA, and often chemically destructive methods of analysis have needed to be utilized for many real-world samples. This work seeks to develop a method that will allow for DNAA to be utilized on samples containing multiple fissile components. Initial efforts, presented here, show that using a multivariate linear regression model to describe the delayed neutron emission profile of an irradiated sample allows for the concurrent determination of fissile nuclides in samples containing both ²³⁵U and ²³⁹Pu, without chemical separations and using only a single counting step.     

Determination of k 0-factors and validation of k 0-INAA for short-lived nuclides

For standardization of k ₀-based instrumental neutron activation analysis, k ₀-factors for short-lived nuclides (half-lives—11 s to 37 min) of elements F, Se, Sc, Al, V, Ti, Cu, Ca, Mg, I, and Cl with respect to gold (¹⁹⁷Au) were determined using pneumatic carrier facility (PCF) at CIRUS reactor of BARC, Mumbai. Characterization of PCF was carried out by cadmium-ratio method using Au and Zr. The experimental k ₀-factors of the isotopes were found to be in good agreement with the recommended k ₀-factors in most of the cases, as evident from the values of % error and U-score at 95% confidence level. The method was validated by determining concentrations of elements through their short-lived nuclides in one type of the synthetic multielement standards (SMELS-I) obtained from SCK-CEN, Belgium. The method was also applied for determination of concentrations of some of the elements in two reference materials of IAEA, SL-3, and SL-1.     

Quantitative Evaluation of Trace Elements in Sediments of the Tamsui River via Instrumental Neutron Activation Analysis

The present study examined concentrations of trace elements in the sediments collected from 31 locations along the banks of Tamsui River by instrumental neutron activation analysis. The Tamsui River is famous for containing a unique area of naturally preserved mangrove in northern Taiwan. It is also the second longest river among the 3 major rivers in Taiwan. A total of 11 nuclides, including Mg, Al, Ti, Mn, Na, Sc, As, Br, La, Fe and Cs, were identified. The categories and measurements of nuclides detected were interpreted according to the sampling locations or chemical attributes characteristics. A dimensionless index (CI) was introduced to explore the quantitative correlation among the detected nuclides. A smaller CI corresponded to a stronger correlation between a pair of nuclides, such that the correlation between the nuclides can be interpreted through a series of quantified indices. The minimum detectable concentration (MDC) for As‐76 was fluctuated around 0.67 ± 0.09 μg/g due to the variations of background counts in various gamma spectra.