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.

Conversion electron spectroscopy of the 59.54 keV transition in 241Am alpha decay.

A windowless Peltier-cooled silicon drift detector (SDD) was used to measure internal conversion electron (ICE) spectra of thin 241Am sources. The ICE peaks associated with the 59.54 keV gamma transition in 237Np were deconvoluted and relative ICE intensities were derived from the fitted peak areas. Corrections were made for energy dependence of the full-energy-peak counting efficiency, based on Monte Carlo simulations. As expected for this anomalous E1 transition, a significant discrepancy was found with the theoretical internal conversion coefficient (ICC) values calculated from the BrIcc database. Penetration effects are known to cause such anomalies in highly retarded transitions. The measured ICE intensities are in good agreement with a specific combination of literature data obtained with magnetic spectrometers.

Linearity check of an ionisation chamber through 99 mTc half-life measurements.

The half-life of 99 mTc was measured at the JRC using the ionisation chamber 'IC1' (type Centronic IG12). The result, T1/2(99 mTc) = 6.00660 (18) h, is in good agreement with literature data. One experiment was performed in IC1's default set-up with the ionisation current being integrated over an air capacitor and read out as a voltage increase over time. This ensured excellent linearity and precision throughout the dynamic range, but the maximum current was limited to 2 nA. In a second test, the current was directly read out with a Keithley 6517 A electrometer. Applying correction factors for the automatic range switching of the electrometer, an acceptable linearity was demonstrated over a range of 12 half-life periods starting at 20 nA. Range switching and autocorrelation of the current readout increase the systematic and random error propagation factors. Piecewise fitting of the decay curve over periods of 6 h yields the same 99 mTc half-life value within 0.04% (0.0025 h) standard deviation over an activity range spanning at least 10 half-life periods (3 orders of magnitude).

Deconvolution of 238,239,240Pu conversion electron spectra measured with a silicon drift detector.

Internal conversion electron (ICE) spectra of thin 238,239,240Pu sources, measured with a windowless Peltier-cooled silicon drift detector (SDD), were deconvoluted and relative ICE intensities were derived from the fitted peak areas. Corrections were made for energy dependence of the full-energy-peak counting efficiency, based on Monte Carlo simulations. A good agreement was found with the theoretically expected internal conversion coefficient (ICC) values calculated from the BrIcc database.

Is decay constant?

Some authors have raised doubt about the invariability of decay constants, which would invalidate the exponential-decay law and the foundation on which the common measurement system for radioactivity is based. Claims were made about a new interaction - the fifth force - by which neutrinos could affect decay constants, thus predicting changes in decay rates in correlation with the variations of the solar neutrino flux. Their argument is based on the observation of permille-sized annual modulations in particular decay rate measurements, as well as transient oscillations at frequencies near 11 year-1 and 12.7 year-1 which they speculatively associate with dynamics of the solar interior. In this work, 12 data sets of precise long-term decay rate measurements have been investigated for the presence of systematic modulations at frequencies between 0.08 and 20 year-1. Besides small annual effects, no common oscillations could be observed among α, ß-, ß+ or EC decaying nuclides. The amplitudes of fitted oscillations to residuals from exponential decay do not exceed 3 times their standard uncertainty, which varies from 0.00023 % to 0.023 %. This contradicts the assertion that 'neutrino-induced' beta decay provides information about the deep solar interior.

Conversion electron spectrometry of Pu isotopes with a silicon drift detector.

An electron spectrometry set-up was built at IRMM consisting of a vacuum chamber with a moveable source holder and windowless Peltier-cooled silicon drift detector (SDD). The SDD is well suited for measuring low-energy x rays and electrons emitted from thin radioactive sources with low self-absorption. The attainable energy resolution is better than 0.5keV for electrons of 30keV. It has been used to measure the conversion electron spectra of three plutonium isotopes, i.e. (238)Pu, (239)Pu, (240)Pu, as well as (241)Am (being a decay product of (241)Pu). The obtained mixed x-ray and electron spectra are compared with spectra obtained with a close-geometry set-up using another SDD in STUK and spectra measured with a Si(Li) detector at IRMM. The potential of conversion electron spectrometry for isotopic analysis of mixed plutonium samples is investigated. With respect to the (240)Pu/(239)Pu isotopic ratio, the conversion electron peaks of both isotopes are more clearly separated than their largely overlapping peaks in alpha spectra.

"Realisation of the becquerel"--reducing the impact of equipment failure.

The goal of the CCRI(II) "Realisation of the becquerel" project is to design a reproducible radioactivity standard which will increase the robustness of the current international reference system for radioactivity measurements. Tests performed with a first prototype ionisation chamber of this project, built in 2005, are presented. Based on experience with the first prototype, a new design was proposed in 2010 aiming at achieving the very ambitious project goals. The article discusses the status of the project and the advantages of the new design.

A magnet system for the suppression of conversion electrons in alpha spectrometry.

A new magnet system has been designed and constructed to reduce coincidence effects between alpha particles and conversion electrons in high-resolution alpha-particle spectrometry. By means of a magnetic field, the conversion electrons are deflected away from the PIPS(®) detector. Compared to existing magnet systems, the new system is not restricted to point sources and can accommodate source diameters up to about 30 mm. Two yokes were built, allowing for configurations with 20 mm or 36 mm distance between the magnets. The effectiveness of both configurations is demonstrated by measuring the conversion electron spectrum of a (237)Np source. The magnet system effectively rejects 93 (7)% of electrons up to 85 keV (36 mm) and 90 (9)% of electrons up to 320 keV (20 mm). It has been successfully applied in the alpha-particle spectrometry of the long-lived nuclides (236)U and (238)U, resulting in significant improvement of the accuracy of alpha emission probabilities.

Alpha-particle emission probabilities of ²³6U obtained by alpha spectrometry.

High-resolution alpha-particle spectrometry was performed with an ion-implanted silicon detector in vacuum on a homogeneously electrodeposited (236)U source. The source was measured at different solid angles subtended by the detector, varying between 0.8% and 2.4% of 4π sr, to assess the influence of coincidental detection of alpha-particles and conversion electrons on the measured alpha-particle emission probabilities. Additional measurements were performed using a bending magnet to eliminate conversion electrons, the results of which coincide with normal measurements extrapolated to an infinitely small solid angle. The measured alpha emission probabilities for the three main peaks - 74.20 (5)%, 25.68 (5)% and 0.123 (5)%, respectively - are consistent with literature data, but their precision has been improved by at least one order of magnitude in this work.

High-resolution alpha-particle spectrometry of ²³8U.

The alpha-particle emission probabilities associated with the three main alpha transitions of (238)U were measured by high-resolution alpha-particle spectrometry. Highly enriched (238)U material was used and its isotopic composition characterised by mass spectrometry. Source production through electrodeposition was optimised to reconcile conflicting demands for good spectral resolution and statistical precision. Measurements were performed at IRMM and CIEMAT for 1-2 years in three different set-ups. A new magnet system was put into use to largely eliminate true coincidence effects with low-energy conversion electrons. Finally the accuracy and precision of the relative emission probabilities for the three transitions - 77.01 (10)%, 22.92 (10)% and 0.068 (10)%, respectively - have been improved significantly.

Half-lives of 221Fr, 217At, 213Bi, 213Po and 209Pb from the 225Ac decay series.

The half-lives of (221)Fr, (217)At, (213)Bi, (213)Po, and (209)Pb were measured by means of an ion-implanted planar Si detector for alpha and beta particles emitted from weak (225)Ac sources or from recoil sources, which were placed in a quasi-2π counting geometry. Recoil sources were prepared by collecting atoms from an open (225)Ac source onto a glass substrate. The (221)Fr and (213)Bi half-lives were determined by following the alpha particle emission rate of recoil sources as a function of time. Similarly, the (209)Pb half-life was determined from the beta particle count rate. The shorter half-lives of (217)At and (213)Po were deduced from delayed coincidence measurements on weak (225)Ac sources using digital data acquisition in list mode. The resulting values: T1/2((221)Fr)=4.806 (6) min, T1/2((217)At)=32.8 (3)ms, T1/2((213)Bi)=45.62 (6)min, T1/2((213)Po)=3.708 (8) µs, and T1/2((209)Pb)=3.232 (5)h were in agreement only with the best literature data.

Decay data measurements on 213Bi using recoil atoms.

In this work, (213)Bi has been separated from an open (225)Ac source by collecting recoil atoms onto a glass plate in vacuum. The activity of such recoil sources has been measured as a function of time, using an ion-implanted planar Si detector in quasi-2π geometry. From these measurements, a new half-life value of T1/2((213)Bi)=45.62 (6)min was derived. Additionally, high-resolution alpha-spectrometry measurements were performed at a solid angle of 0.4% of 4πsr, to verify the energies and emission probabilities of the α-emissions from (213)Bi. Using (225)Ac, (221)Fr, (217)At and (213)Po peaks as reference peaks, the measured (213)Bi α-peak energies at Eα,0=5878 (4)keV and Eα,1=5560 (4)keV were about 10keV higher than validated data. The relative α-particle emission probabilities of (213)Bi, Pα,0=0.9155 (11) and Pα,1=0.0845 (11), and the (213)Bi alpha branching factor, Pα=1-Pß=2.140 (10)%, are compatible with recommended values, but have a higher accuracy.

Measurement of the 226Th and 222Ra half-lives.

The half-lives of (226)Th and (222)Ra were measured by counting alpha-particle emissions from sources as a function of time. The (226)Th sources were prepared from an open (230)U source, capturing recoil atoms after alpha-particle decay on glass disks or even directly onto a detector. Similarly, the (222)Ra sources were obtained by self-transfer of recoil atoms from (226)Th sources. The activity measurements were performed in (nearly-)2π geometry with an ion-implanted silicon detector. The decay curves were analysed in different ways, incl. moment analysis, trying to avoid the pitfalls of bias of least-squares fits to Poisson distributed data. The observed half-life values are T(1/2)((226)Th)=30.70 (3) min and T(1/2)((222)Ra)=33.6 (4) s. Literature values show some inconsistency.

Measurements of the half-life of 214Po and 218Rn using digital electronics.

The half-lives of (214)Po and (218)Rn have been measured. The radionuclides were produced in the decay of a (230)U source and the emitted alpha-particles were measured in nearly-2π geometry with an ion-implanted planar silicon detector. The data acquisition was performed with a digitiser operated in list mode, saving the energy and time of detection (10 ns precision timestamp) of each event. The half-lives were deduced from the time differences between the alpha-decays populating the nuclide of interest and those corresponding to its decay. Different methods were applied, based on delayed coincidence counting and time-interval distribution analysis. The resulting half-lives are 33.75 (15) ms for (218)Rn and 164.2 (6) µs for (214)Po, both in agreement with some of the literature values, and obtained with higher precision in this work.

High-resolution alpha-particle spectrometry of the 230U decay series.

High-resolution alpha-particle spectrometry was performed on the (230)U decay series. A (230)U source was prepared on a stainless steel disc by electrodeposition in an ammonium nitrate solution. Spectrometry of the alpha-particle energy spectrum was performed with ion-implanted planar silicon detectors in vacuum. A set of alpha emission probabilities is presented for (230)U and (226)Th. The measured peak intensities were corrected mathematically for coincidental detection of alpha-particles and conversion electrons emitted in the same decay. A good agreement with literature data was observed. The uncertainty budget and the correlation matrix are presented. The validity of the alpha-particle energies was tested and could be confirmed for most peaks within a few keV, but discrepancies were found for the 2nd peak of (226)Th and the main peak of (218)Rn.

Measurement of the 225Ac half-life.

The (225)Ac half-life was determined by measuring the activity of (225)Ac sources as a function of time, using various detection techniques: α-particle counting with a planar silicon detector at a defined small solid angle and in a nearly-2π geometry, 4πα+ß counting with a windowless CsI sandwich spectrometer and with a pressurised proportional counter, gamma-ray spectrometry with a HPGe detector and with a NaI(Tl) well detector. Depending on the technique, the decay was followed for 59-141 d, which is about 6-14 times the (225)Ac half-life. The six measurement results were in good mutual agreement and their mean value is T(1/2)((225)Ac)=9.920 (3)d. This half-life value is more precise and better documented than the currently recommended value of 10.0 d, based on two old measurements lacking uncertainty evaluations.

Measurement of the 230U half-life.

The (230)U half-life was determined by measuring the decay curve of (230)U sources by various nuclear detection techniques: α-particle counting at a defined small solid angle; 4πα+ß counting with a windowless CsI sandwich spectrometer, a liquid scintillation counter and a pressurised proportional counter; gamma-ray spectrometry with a HPGe detector and nearly-2π α-particle counting with an ion-implanted silicon detector. Depending on the technique, the decay was followed for 100-200 d, which is 5-10 times the (230)U half-life. The measurement results of the various techniques were in good mutual agreement. The mean value, T(1/2)((230)U)=20.23 (2) d, is lower than the literature value which is based on one measurement in 1948 and resulted in a half-life value of 20.8d without statement of uncertainty. A correction for the ingrowth of the long-lived (210)Pb and its daughter products may have been overlooked in the past.

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.

Measurement of the 109Cd half-life.

The half-life of (109)Cd was measured by following the decay of sources from a radiochemically pure solution with two different measuring systems: an ionisation chamber and a high-purity germanium (HPGe) detector. The measurements were performed over a period of 3.6 years, i.e. about 2.8 half-lives of (109)Cd. The resulting half-life values and detailed uncertainty budgets (k=1) are presented for both systems. The result obtained with the ionisation chamber, 462.36 (33) days, and the one obtained with the HPGe detector, 461.92 (76) days, are mutually consistent. The weighted mean of our measured values, T(1/2)((109)Cd)=462.29 (30) days, is consistent with the currently recommended values of 461.4 (12) days (Schönfeld and Dersch, 2004; IAEA, 2007) and 462.0 (3) days (Xiaolong et al., 2010). From a set of selected experimental values published after 1970, a "partially weighted mean" (Pommé and Spasova, 2008) of T(1/2)((109)Cd)=462.36 (39) days was calculated. More measurements are needed to resolve the discrepancies among literature data and to reduce the final uncertainty on the (109)Cd half-life.

Measurement of the 177Lu half-life.

The half-life of (177)Lu was measured by following the decay of sources with an ionisation chamber and with a liquid scintillation counter over a period of 85 and 42 days, respectively. The detector signals showed three major components: decay of (177)Lu, decay of (177m)Lu and the background signal. The half-life value, T(1/2)((177)Lu)=6.6465 (50)d, was obtained by a least-squares fit of two exponential decay functions and a constant background to the experimental data. The data was corrected for decay during the measurements. Residuals of the fit and uncertainty budgets are presented in this paper. The result is in agreement with three out of seven previously published measurement results and the currently recommended value of 6.647 (4) d (Kondev, 2002). A new value of T(1/2)((177)Lu)=6.6465 (32) d was obtained from a weighted mean of our results with the selected literature data.