W.M. van Wyngaardt

Fe-55 activity measurements at the NMISA revisited.

Twenty years ago South Africas Radioactivity Standards Laboratory (now operated by the NMISA) was the first to measure the activity of (55)Fe by combining the triple-to-double coincidence ratio (TDCR) liquid scintillation method with theoretical efficiency formulae. The extracted activity was however found to be consistently low by about 6%. Due to improvements in both the counting system and analysis technique, it was decided to re-examine the method as applied at the NMISA. The latest results are presented and discussed, particularly with regard to a quantitative study into which vial type is better suited to obtaining accurate (55)Fe activity measurements.

Comparison of triple-to-double coincidence ratio (TDCR) efficiency calculations and uncertainty assessments for 99Tc

A comparison exercise for data analysis was recently conducted by the Liquid Scintillation Counting Working Group (LSCWG) of the International Committee on Radionuclide Metrology (ICRM) to evaluate the uncertainties involved in applying different analysis methodologies (including computer programs) for the triple-to-double coincidence ratio (TDCR) method. The goals of the comparison were to (1) study differences in calculation results from different TDCR analysis programs, (2) investigate differences in analysis techniques and uncertainty assessment philosophies between laboratories, and (3) study the effect of not taking asymmetry of photomultiplier tube (PMT) efficiencies into account on the calculated activity. To achieve this, a single set of TDCR data for the pure beta emitter (99)Tc, was distributed to the participants, who analyzed the data according to their normal procedures and report the activity concentration of the (99)Tc solution from their results. The results indicate that the presently used programs are generally able to calculate the same activity values, assuming that the correct input parameters are used and that not taking PMT asymmetry into account in the calculations can lead to significant (0.6% for (99)Tc) errors in reported results. The comparison also highlighted the need for a more rigorous approach to estimating and reporting uncertainties.

On decay constants and orbital distance to the Sun—part III: beta plus and electron capture decay

The hypothesis that seasonal changes in proximity to the Sun cause variation of decay constants at permille level has been tested for radionuclides disintegrating through electron capture and beta plus decay. Activity measurements of 22Na, 54Mn, 55Fe, 57Co, 65Zn, 82+85Sr, 90Sr, 109Cd, 124Sb, 133Ba, 152Eu, and 207Bi sources were repeated over periods from 200 d up to more than four decades at 14 laboratories across the globe. Residuals from the exponential nuclear decay curves were inspected for annual oscillations. Systematic deviations from a purely exponential decay curve differ from one data set to another and appear attributable to instabilities in the instrumentation and measurement conditions. Oscillations in phase with Earths orbital distance to the sun could not be observed within 10−4–10−5 range precision. The most stable activity measurements of β + and EC decaying sources set an upper limit of 0.006% or less to the amplitude of annual oscillations in the decay rate. There are no apparent indications for systematic oscillations at a level of weeks or months.

On decay constants and orbital distance to the Sun—part II: beta minus decay

Claims that proximity to the Sun causes variations of decay constants at the permille level have been investigated for beta-minus decaying nuclides. Repeated activity measurements of H-3, C-14, Co-60, Kr-85, Sr-90, Sb-124, Cs-134, Cs-137, and Eu-154 sources were performed over periods of 259 d up to 5 decades at various nuclear metrology institutes. Residuals from the exponential decay curves were inspected for annual oscillations. Systematic deviations from a purely exponential decay curve differ in amplitude and phase from one data set to another and appear attributable to instabilities in the instrumentation and measurement conditions. Oscillations in phase with Earths orbital distance to the Sun could not be observed within 10(-4)-10(-5) range precision. The most stable activity measurements of beta-decaying sources set an upper limit of 0.003%-0.007% to the amplitude of annual oscillations in the decay rate. There are no apparent indications for systematic oscillations at a level of weeks or months.

On decay constants and orbital distance to the Sun - Part I: Alpha decay

Claims that proximity to the Sun causes variation of decay constants at permille level have been investigated for alpha decaying nuclides. Repeated decay rate measurements of Po-209, Ra-226, Th-228, U-230, and Am-241 sources were performed over periods of 200 d up to two decades at various nuclear metrology institutes around the globe. Residuals from the exponential decay curves were inspected for annual oscillations. Systematic deviations from a purely exponential decay curve differ in amplitude and phase from one data set to another and appear attributable to instabilities in the instrumentation and measurement conditions. The most stable activity measurements of alpha decaying sources set an upper limit between 0.0006% and 0.006% to the amplitude of annual oscillations in the decay rate. There are no apparent indications for systematic oscillations at a level of weeks or months. Oscillations in phase with Earths orbital distance to the sun could not be observed within 10(-5)-10(-6) range precision.

Results of an international comparison for the activity measurement of 177Lu

An international Key Comparison of (177)Lu has recently been carried out. Twelve laboratories performed assays for radioactivity content on aliquots of a common master solution of (177)Lu, leading to eleven results submitted for entry into the Key Comparison Database of the Mutual Recognition Arrangement. A proposed Comparison Reference Value (CRV) was calculated to be 3.288(4)MBq/g using all eleven results. Degrees of equivalence and their uncertainties were calculated for each laboratory based on the CRV. Most of the values reported by the participating laboratories were within 0.6% of the CRV.

Evidence against solar influence on nuclear decay constants

The hypothesis that proximity to the Sun causes variation of decay constants at permille level has been tested and disproved. Repeated activity measurements of mono-radionuclide sources were performed over periods from 200 days up to four decades at 14 laboratories across the globe. Residuals from the exponential nuclear decay curves were inspected for annual oscillations. Systematic deviations from a purely exponential decay curve differ from one data set to another and are attributable to instabilities in the instrumentation and measurement conditions. The most stable activity measurements of alpha, beta-minus, electron capture, and beta-plus decaying sources set an upper limit of 0.0006% to 0.008% to the amplitude of annual oscillations in the decay rate. Oscillations in phase with Earth’s orbital distance to the Sun could not be observed within a 10−6 to 10−5 range of precision. There are also no apparent modulations over periods of weeks or months. Consequently, there is no indication of a natural impediment against sub-permille accuracy in half-life determinations, renormalisation of activity to a distant reference date, application of nuclear dating for archaeology, geo- and cosmochronology, nor in establishing the SI unit becquerel and seeking international equivalence of activity standards.

Absolute activity of 133Ba by liquid scintillation coincidence counting using the 4π(e,X)-γ extrapolation technique

The Technical Committee for Ionizing Radiation (TCRI) of the Asia Pacific Metrology Programme (APMP) recently organized a regional key comparison of activity measurements of the radionuclide (133)Ba. This paper reports on absolute measurements made at the National Metrology Institute of South Africa (NMISA) by the coincidence extrapolation technique, with liquid scintillation counting (LSC) comprising the 4pi channel. A detection efficiency analysis was undertaken to predict the maximum efficiency likely to be achieved and to confirm that the method does indeed provide the source disintegration rate for (133)Ba. Various experimental and data analysis difficulties to be aware of are discussed in the paper.

Further investigations of a simple counting technique for measuring mixtures of two pure β-emitting radionuclides

A simple liquid scintillation counting technique to measure the activity composition of a mixture containing two known pure beta-emitting radionuclides was recently developed at the NMISA. The method has been applied to various two-component mixtures of (32)P, (33)P and (35)S, primarily to gauge the effect of spectral energy differences on the methods ability to extract the individual activities. Excellent results were obtained for mixtures of (33)P and (35)S, radionuclides with similar, low beta energies. Mixtures containing the high-energy beta-emitter (32)P were more difficult to resolve, although quenching of the counting sources with CHCl(3) improved mixture resolution.

Accurate activity measurement of Lu-177 by the liquid scintillation 4πβ-γ coincidence counting technique.

This paper reports on absolute measurements made at the NMISA by the 4π[LS]β-γ coincidence extrapolation technique, which formed part of a key comparison of activity measurements of the radionuclide lutetium-177, a beta-gamma emitter. A detection efficiency analysis based on the decay scheme indicated that the coincidence extrapolation method is feasible for extracting the source disintegration rate of (177)Lu. A simulation was undertaken utilizing the efficiency equations to give an indication of the expected variation of the source count rate with efficiency for different gamma-ray windows. Both the simulation and experiment indicated that the window giving the highest counting efficiency was centered about the 208.4 keV photopeak, with the data showing linear variation in the upper efficiency range. The extracted activity concentration of the (177)Lu solution proved to be highly accurate, being higher than the proposed comparison reference value by 0.15%, well within one standard uncertainty (σ=0.26%) as specified by the NMISA.