Evaluation of different methods for measuring 89Sr and 90Sr: Measurement uncertainty for the different methods as a function of the activity ratio.

In case of a radiological emergency situation involving e.g. fission of uranium or plutonium, analysis of radioactive strontium will be of importance. The primary radionuclides of interest are 90Sr, its progeny 90Y and 89Sr. A few days following an event, 89Sr will be the predominant radioisotope of strontium. Most methods found in the literature are valid and applicable when measuring 90Sr, but when samples contain both 89Sr/90Sr interference problematics arise. How these interferences are dealt with will have an effect on the uncertainty of the 90Sr determination. This work aims at evaluating three measurement approaches, all mentioned in the literature, with respect to the measurement uncertainty when determining 90Sr in an emergency preparedness situation and to propose a suitable measurement strategy.

Comparing results of X-ray diffraction, µ-Raman spectroscopy and neutron diffraction when identifying chemical phases in seized nuclear material, during a comparative nuclear forensics exercise.

This work presents the results for identification of chemical phases obtained by several laboratories as a part of an international nuclear forensic round-robin exercise. In this work powder X-ray diffraction (p-XRD) is regarded as the reference technique. Neutron diffraction produced a superior high-angle diffraction pattern relative to p-XRD. Requiring only small amounts of sample, µ-Raman spectroscopy was used for the first time in this context as a potentially complementary technique to p-XRD. The chemical phases were identified as pure UO2 in two materials, and as a mixture of UO2, U3O8 and an intermediate species U3O7 in the third material.

Application of a Monte Carlo method to the uncertainty assessment in in situ gamma-ray spectrometry.

In situ gamma-ray spectrometry has since the introduction of portable germanium detectors been a widely used method for the assessment of radionuclide ground deposition activity levels. It is, however, a method that is most often associated with fairly large and, more important, poorly known combined measurement uncertainties. In this work an uncertainty analysis of in situ gamma ray spectrometry in accordance with the Guide to the Expression of Uncertainty in Measurements is presented. The uncertainty analysis takes into account uncertainty contributions from the calibration of the detector system, the assumed activity distribution in soil, soil density, detector height and air density. As a result, measurement results from in situ gamma spectrometry will serve as a better basis for decision-making in e.g. radiological emergencies.

Time optimization of 90Sr determinations: sequential measurement of multiple samples during decay of 90Y.

This work presents an optimized method for the determination of multiple samples containing 90Sr when its daughter 90Y is measured after chemical separation and in sequence, i.e. during its decay. Consequently the measurement times will increase for each subsequent sample, since there has been a longer time for decay before measurement. Compared to a previously published approach, when 90Y is measured during its ingrowth, the gain in total analysis time (time for ingrowth+ summation of measurement times) is not that large, particularly not for low background instruments. However, results for a large part of the samples can be delivered earlier.

Time optimization of (90)Sr measurements: Sequential measurement of multiple samples during ingrowth of (90)Y.

The aim of this paper is to contribute to a more rapid determination of a series of samples containing (90)Sr by making the Cherenkov measurement of the daughter nuclide (90)Y more time efficient. There are many instances when an optimization of the measurement method might be favorable, such as; situations requiring rapid results in order to make urgent decisions or, on the other hand, to maximize the throughput of samples in a limited available time span. In order to minimize the total analysis time, a mathematical model was developed which calculates the time of ingrowth as well as individual measurement times for n samples in a series. This work is focused on the measurement of (90)Y during ingrowth, after an initial chemical separation of strontium, in which it is assumed that no other radioactive strontium isotopes are present. By using a fixed minimum detectable activity (MDA) and iterating the measurement time for each consecutive sample the total analysis time will be less, compared to using the same measurement time for all samples. It was found that by optimization, the total analysis time for 10 samples can be decreased greatly, from 21h to 6.5h, when assuming a MDA of 1Bq/L and at a background count rate of approximately 0.8cpm.

Characterization of strong (241)Am sources.

Gamma ray spectra of strong (241)Am sources may reveal information about the source composition as there may be other radioactive nuclides such as progeny and radioactive impurities present. In this work the possibility to use gamma spectrometry to identify inherent signatures in (241)Am sources in order to differentiate sources from each other, is investigated. The studied signatures are age, i.e. time passed since last chemical separation, and presence of impurities. The spectra of some sources show a number of Doppler broadened peaks in the spectrum which indicate the presence of nuclear reactions on light elements within the sources. The results show that the investigated sources can be differentiated between by age and/or presence of impurities. These spectral features would be useful information in a national nuclear forensics library (NNFL) in cases when the visual information on the source, e.g. the source number, is unavailable.

Distribution and transport of radionuclides in a boreal mire--assessing past, present and future accumulation of uranium, thorium and radium.

The spatial distribution of (238)U, (226)Ra, (40)K and the daughters of (232)Th, (228)Ra and (228)Th, were measured in a small mire in northern Sweden. High activity concentrations of (238)U and (232)Th (up to 41 Bq (238)U kg(-1)) were observed in parts of the mire with a historical or current inflow of groundwater from the surrounding till soils, but the activities declined rapidly further out in the mire. Near the outlet and in the central parts of the mire the activity concentrations were low, indicating that uranium and thorium are immobilized rapidly upon their entering the peat. The (226)Ra was found to be more mobile with high activity concentrations further out into the mire (up to 24 Bq kg(-1)), although the central parts and the area near the outlet of the mire still had low activity concentrations. Based on the fluxes to and from the mire, it was estimated that approximately 60-70% of the uranium and thorium entering the mire currently is retained within it. The current accumulation rates were found to be consistent with the historical accumulation, but possibly lower. Since much of the accumulation still is concentrated to the edges of the mire and the activities are low compared to other measurements of these radionuclides in peat, there are no indications that the mire will be saturated with respect to radionuclides like uranium, thorium and radium in the foreseen future. On the contrary, normal peat growth rates for the region suggest that the average activity concentrations of the peat currently may be decreasing, since peat growth may be faster than the accumulation of radionuclides. In order to assess the total potential for accumulation of radionuclides more thoroughly it would, however, be necessary to also investigate the behaviour of other organophilic elements like aluminium, which are likely to compete for binding sites on the organic material. Measurements of the redox potential and other redox indicators demonstrate that uranium possibly could be reduced in parts of the mire. The results of the study suggest that this mire currently is, and historically has been, an important sink for radionuclides and that it most likely will continue to be so for a long time to come.

Evaluation of Monte Carlo-based calibrations of HPGe detectors for in situ gamma-ray spectrometry.

The aim of this work was to evaluate the use of Monte Carlo-based calibrations for in situ gamma-ray spectrometry. We have performed in situ measurements at five different sites in Sweden using HPGe detectors to determine ground deposition activity levels of (137)Cs from the 1986 Chernobyl accident. Monte Carlo-calculated efficiency calibration factors were compared with corresponding values calculated using a more traditional semi-empirical method. In addition, results for the activity ground deposition were also compared with activity densities found in soil samples. In order to facilitate meaningful comparisons between the different types of results, the combined standard uncertainty of in situ measurements was assessed for both calibration methods. Good agreement, both between the two calibration methods, and between in situ measurements and soil samples, was found at all five sites. Uncertainties in in situ measurements for the given measurement conditions, about 20 years after the fallout occurred, were found to be in the range 15-20% (with a coverage factor k=1, i.e. with a confidence interval of about 68%).

Uncertainty in HPGe detector calibrations for in situ gamma-ray spectrometry.

Semi-empirical methods are often used for efficiency calibrations of in situ gamma-ray spectrometry measurements with high-purity germanium detectors. The intrinsic detector efficiency is experimentally determined for different photon energies and angles of incidence, and a suitable expression for the efficiency is fitted to empirical data. In this work, the combined standard uncertainty of such an efficiency function for two detectors was assessed. The uncertainties in individual efficiency measurements were found to be about 1.9 and 3.1% (with a coverage factor k = 1, i.e. with a confidence interval of about 68%) for the two detectors. The main contributions to these uncertainties were found to originate from uncertainties in source-to-detector distance, source activity and full-energy peak count rate. The standard uncertainties of the fitted functions were found to be somewhat higher than the uncertainty of individual data points, i.e. 5.2 and 8.1% (k = 1). With the introduction of a new expression for the detector efficiency, these uncertainties were reduced to 3.7 and 4.2%, i.e. with up to a factor of two. Note that this work only addresses the uncertainty in the determination of intrinsic detector efficiency.