B.R.S. Simpson

Comparison of activity concentration measurement of 63Ni and 55Fe in the framework of the EUROMET 297 project

Abstract Eleven laboratories participated in an intercomparison of activity concentration measurements using liquid scintillation counting (LSC) for the standardization of 63Ni and 55Fe in the frame of the EUROMET project No. 297 and under the co-ordination of LPRI. The purpose of this action was to compare the main LSC activity concentration measurement methods currently used in radioactive metrology, and to exchange models and ideas on LSC. This paper presents a summary of the results reported by the participant laboratories and an overview of the measurement methods used.

International Comparison of Measurements of the Specific Activity of Tritiated Water

Abstract An international comparison of measurements of the specific activity of tritiated water has been carried out under the auspices of the ICRM Radionuclide Techniques Working Group. The comparison, in which nine laboratories participated, involved the measurement of tritiated water samples of unknown specific activity at up to three different activity levels. The results of the comparison are reported, together with information on the measurement techniques employed and the measurement uncertainties.

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.

International comparison CCRI(II)-S7 on the analysis of uncertainty budgets for 4πβγ coincidence counting

Detailed uncertainty reporting is imperative for proficiency tests and comparison exercises because uncertainties need to be comparable and trusted by all the participants. Even though participants do their best to follow the Guide to the Expression of Uncertainty in Measurement, ambiguities and divergences about uncertainty evaluation remain. Consequently, to analyze the situation, the CCRI (II) Uncertainties Working Group proposed a comparison exercise (CCRI(II)-S7) about the uncertainty evaluation of a relatively simple primary activity measurement: the standardization of a 60Co source by coincidence counting. To be able to understand how various NMIs calculate coincidence counting uncertainties, our study focused on two of the dominant uncertainty components commonly quoted for 4πβ-γ coincidence counting in the International Reference System (SIR) submissions and Key Comparison exercises: efficiency-extrapolation and weighing. Participants from twelve different laboratories were sent the same set of measurement data from the analysis of a 60Co solution standardized at the National Physical Laboratory (NPL). Our study demonstrated the extent of the different interpretations of the uncertainty components. Some factors causing large discrepancies were isolated and are discussed. Further studies of other techniques using a similar approach would be beneficial for the metrology community. Main text. To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/. The final report has been peer-reviewed and approved for publication by the CCRI, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).