Youcef Nedjadi

A new measurement of the half-life of 166mHo

The work presented here is a new and precise measurement of the half-life of (166m)Ho by determining the activity concentration, using an ionisation chamber calibrated for this nuclide, and measuring the number of (166m)Ho atoms using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Since the isotope (166)Er interferes with the mass spectrometric measurement, Er has to be eliminated from the (166m)Ho radioactive solution. The elimination was achieved using ion-exchange chromatography with the cation exchange resin Dowex AG 50W-X8 and 2-Hydroxybutanoic acid as the mobile phase. After a first transit through the chromatographic column, the purified (166m)Ho eluate was spiked with natural Er to get a resulting Er isotopic composition close to that of natural Er at better than 99.5%, and then it underwent two further separations to eliminate the Er. The activity concentration of this Er-free radioactive (166m)Ho solution was measured in our reference ionisation chamber calibrated for this nuclide by means of the 4πβ(PC)-γ and 4πβ(PS)-4πγ coincidence techniques and integral counting with a well-type NaI(Tl) detector and Monte Carlo efficiencies. An aliquot of this standardized solution was sent to the Paul Scherrer Institute (PSI) for mass concentration determination using an isotope dilution MC-ICP-MS approach. The mass concentration of (166m)Ho in this solution was determined with 0.25% relative standard uncertainty. This value was corroborated by two other independent measurements. The new half-life of (166m)Ho, 1132.6(39) years (k=1), is compatible with the value determined in 1965, but is 5.6% shorter and about 43 times more precise.

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.

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).

International exercise on 124Sb activity measurements.

An international exercise, registered as EUROMET project no. 907, was launched to measure both the activity of a solution of (124)Sb and the photon emission intensities of its decay. The same solution was sent by LNE-LNHB to eight participating laboratories. In order to identify possible biases, the participants were asked to use all possible activity measurement methods available in their laboratory and then to determine their reference value for comparison. Thus, measurement results from 4pibeta-gamma coincidence/anti-coincidence counting, CIEMAT/NIST liquid-scintillation counting, 4pigamma counting with well-type ionization chambers and well-type crystal detectors were given. The results are compared and show a maximum discrepancy of about 1.6%: possible explanations are proposed.

Primary activity measurements with a 4πβ-4πγ coincidence counting system.

The radioactive concentrations of (166m)Ho, (134)Cs and (133)Ba solutions have been standardised using a 4πβ-4πγ coincidence counting system we have recently set up. The detection in the beta channel is performed using various geometries of a UPS-89 plastic scintillator optically coupled to a selected low-noise 1in. diameter photomultiplier tube. The light-tight thin capsule that encloses this beta detector is housed within the well of a 5in.×5in. NaI(Tl) monocrystal detector. The beta detection efficiency can be varied either by optical filtering or electronic discrimination when the electrons loose all their energy in the plastic scintillator. This 4πβ-4πγ coincidence system improves on our 4πβ(PC)-γ system in that its sample preparation is less labour intensive, it yields larger beta- and gamma-counting efficiencies thus enabling the standardisation of low activity sources with good statistics in reasonable time, and it makes standardising short-lived radionuclides easier. The resulting radioactive concentrations of (166m)Ho, (134)Cs and (133)Ba are found to agree with those measured with other primary measurement methods thus validating our 4πβ-4πγ coincidence counting system.

Activity measurements of 18F and 90Y with commercial radionuclide calibrators for nuclear medicine in Switzerland

The activity of radiopharmaceuticals in nuclear medicine is measured before patient injection with radionuclide calibrators. In Switzerland, the general requirements for quality controls are defined in a federal ordinance and a directive of the Federal Office of Metrology (METAS) which require each instrument to be verified. A set of three gamma sources (Co-57, Cs-137 and Co-60) is used to verify the response of radionuclide calibrators in the gamma energy range of their use. A beta source, a mixture of (90)Sr and (90)Y in secular equilibrium, is used as well. Manufacturers are responsible for the calibration factors. The main goal of the study was to monitor the validity of the calibration factors by using two sources: a (90)Sr/(90)Y source and a (18)F source. The three types of commercial radionuclide calibrators tested do not have a calibration factor for the mixture but only for (90)Y. Activity measurements of a (90)Sr/(90)Y source with the (90)Y calibration factor are performed in order to correct for the extra-contribution of (90)Sr. The value of the correction factor was found to be 1.113 whereas Monte Carlo simulations of the radionuclide calibrators estimate the correction factor to be 1.117. Measurements with (18)F sources in a specific geometry are also performed. Since this radionuclide is widely used in Swiss hospitals equipped with PET and PET-CT, the metrology of the (18)F is very important. The (18)F response normalized to the (137)Cs response shows that the difference with a reference value does not exceed 3% for the three types of radionuclide calibrators.

Update of the BIPM comparison BIPM.RI(II)-K1.Ho-166m activity measurements to include the IRA and the NPL and a re-evaluation of the degrees of equivalence for the APMP.RI(II)-K2.Ho-166m comparison

The IRA and the NPL have submitted ampoules of 166Hom to the International Reference System (SIR) for activity comparison at the Bureau International des Poids et Mesures, thus becoming the third and fourth participants since 1989. The five samples of known activity of 166Hom now recorded in the SIR have activities between about 70 kBq and 500 kBq. The new results have enabled a re-evaluation of the key comparison reference value, and the degrees of equivalence between each equivalent activity measured in the SIR and the key comparison reference value (KCRV) have been calculated. The results are given in the form of a matrix for these four NMIs together with the recalculated degrees of equivalence of an APMP regional comparison held in 2000, comparison identifier APMP.RI(II)-K2.Ho-166m for six other NMIs. A graphical presentation is also given. 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 Section II, according to the provisions of the CIPM Mutual Recognition Arrangement (MRA).