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The aim of this work was to prepare reference radon emanation sources traceable to primary standards to be used for radon-in-air as well as radon-in-water experiments. The feasibility of making stable radon emanation sources by drop deposition and chemisorption was studied. Experimental emanation coefficients for sources made by drop deposition and chemisorption ranged from 0.10 to 0.74 and from 0.18 to 0.25, respectively. These relatively low emanation coefficient values suggest that further method developments would be desirable. Proposals are made to improve chemisorption yield during source preparation and to obtain more accurate measurements on radon emanation coefficient.

The half-life of 243Am has been measured by an absolute and a relative method, i.e. by determining the specific activity of 243Am and the specific activity ratio with 241Am. A mixed 241,243Am reference material was produced and certified for its americium mass content and its isotope amount ratios. The characterisation of the mass content of 243Am was established by isotope dilution mass spectrometry using an 241Am spike, produced from highly enriched 241Pu material. The isotope amount ratios n(241Am)/n(243Am) and n(242mAm)/n(243Am) were measured by thermal ionisation mass spectrometry. Activity measurements were performed by alpha-particle counting at a defined solid angle, as well as high-resolution alpha-particle spectrometry. From the 243Am/241Am activity and isotopic amount ratios, a value of 16.988 (24) was derived for the 243Am/241Am half-life ratio. Using a value of 432.6 (6) a for the 241Am half-life, the corresponding 243Am half-life value, 7349 (15) a, is in good agreement with the result obtained from the absolute method, 7342 (14) a. The mean value, 7345 (14) a, agrees well with data from literature and lowers the relative standard uncertainty to 0.2%.

The emission probabilities of γ rays produced in the 227Ac decay series were determined by high-resolution γ-ray spectrometry of sources with standardised activity. The sources were prepared quantitatively on glass discs by drop deposition of a solution with 227Ac in radioactive equilibrium with its daughter nuclides. Their activity was measured by a primary standardisation technique based on alpha-particle counting at a defined low solid angle. Four laboratories performed γ-ray spectrometry and derived absolute γ-ray intensities. Mean values were calculated and compared with literature data and the currently recommended evaluated data. New values on certain γ-ray emission probabilities are proposed. © 2018 The Authors

Sturrock et al. have published a “rebuttal” to a paper by Pomme et al. who refuted their claim that variations in a radon decay experiment at the Geological Survey of Israel (GSI) can be associated with solar rotation. Sturrock et al. misinterpret the variability of the decay rates in the gamma counter to assert influences by solar and cosmic neutrinos on beta decay and draw unsubstantiated conclusions about solar dynamics. Evidence suggests that the radon measurements were susceptible to solar irradiance and rainfall, whereas there is no indication that radioactive decay is influenced by the solar neutrino flux. In this reply to the rebuttal, the arguments raised by Sturrock et al. are scrutinised.

Accurate measurements were performed of the photon emission probabilities following the α decay of 235U to 231Th. Sources of highly enriched 235U were characterised in terms of isotopic composition by mass spectrometry and their activities were standardised by means of alpha-particle counting at a low defined solid angle. The standardised sources were subsequently measured by high-resolution γ-ray spectrometry with calibrated high-purity germanium detectors to determine the photon emission probabilities. Four laboratories participated in this work and reported emission probabilities for 33 γ-ray lines. Most of them agree with previously published evaluated data. In addition, new values are proposed for γ-lines which have been measured only once in the past. © 2017 The Authors

Claims were made by Sturrock et al. that radioactive decay can be induced by interaction of the nucleus with solar neutrinos and that cyclic modulations in decay rates are indicative of the dynamics of the solar interior. They analysed a series of measurements of gamma radiation associated with the emanation and decay of radon in a sealed container at the Geological Survey of Israel (GSI) laboratory. The integral count rates in the NaI detector showed strong variations in time of year and time of day. From time-series analysis, Sturrock et al. claim the presence of small oscillations at frequencies in a range between 7.4 a−1 and 12.5 a−1, which they speculatively associated with rotational influence on the solar neutrino flux. In this work, it is argued that the GSI radon measurements are unsuited for studying the variability of decay constants, because the data are strongly influenced by environmental conditions, such as solar irradiance and rainfall. At the JRC and PTB, decay rate measurements of the radon decay chain were performed with ionisation chambers, gamma-ray spectrometers and an alpha spectrometer. No deviation from the exponential-decay law was observed. The existence of cyclic variations in the decay constants is refuted, as well as the concept of measuring solar rotation through radioactive decay.

High-resolution alpha-particle spectrometry was performed to determine the main alpha-particle emission probabilities in the decay of 226Ra. Thin, homogeneous sources were prepared by electrodeposition on stainless steel disks. Alpha spectra with an energy resolution of 20keV were obtained in three laboratories and analysed with different deconvolution algorithms. In two set-ups, a magnet system was used to deflect conversion electrons to avoid their coincidental detection with the alpha particles. Spectra taken at close range without a magnet system yielded biased results which cannot be fully compensated by statistical corrections for coincidence summing. The derived emission probabilities of the three main alpha decays are 94.07 (1)%, 5.93 (1)%, and 0.0059 (15)%, respectively. They are in excellent agreement with calculated values derived from the P(γ+ce) decay scheme balance, which solves the existing discrepancy problem with two previous direct measurements published in literature.

The nuclide

A windowless Peltier-cooled silicon drift detector (SDD) was used to measure internal conversion electron (ICE) spectra of thin

International audience; 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 Na-22, Mn-54, Fe-55, Co-57, Zn-65, Sr82+85, Sr-90, Cd-109, Sb-124, Ba-133, Eu-152, and Bi-207 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 Earth's orbital distance to the sun could not be observed within 10(-4)-10(-5) range precision. The most stable activity measurements of beta(+) 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.

The emission probabilities of γ rays produced in the

The uncertainty in neutron cross section values strongly depends on the quality and characteristics of the deposited actinide films which are used as “targets” in the nuclear experiments. Until recently, at the Joint Research Centre in Geel (JRC-Geel), mass and areal densities of actinide layers were determined by measuring activity (using alpha-particle counting), isotopic composition (using thermal ionisation mass spectrometry) and diameter.In this study a series of 238U deposits, prepared by molecular plating and vacuum deposition on different substrates, were characterized with additional non-destructive and destructive analysis techniques. The quality of the deposits was investigated by autoradiography, high-resolution alpha-particle spectrometry, and scanning electron microscopy. The elemental composition was determined by x-ray photoelectron spectroscopy and inductively coupled plasma mass spectrometry. The latter technique was also applied on the U3O8 starting material and the converted UF4 powder. This paper compares the quality and morphology of deposited 238U films prepared by molecular plating and vacuum deposition on various backings, including their elemental composition determined by different characterization techniques. Also discussed are problems in target preparation and characterization.

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.

Internal conversion electron (ICE) spectra of thin

Nuclear decay data measurements were performed in the frame of a EURAMET project. Two specific goals were addressed: (1) High-precision measurements of 238U alpha-particle emission probabilities and (2) experimental characterization of the shape of beta spectra using cryogenic detectors. In the paper, specific lessons learned from the metrological work are highlighted. This includes effects of source preparation on the quality of alpha and beta spectrometry, the influence of exchange effects on beta spectra and the use of a magnet system to eliminate coincidence effects by conversion electrons in alpha-particle spectra., JRC.D.4-Standards for Nuclear Safety, Security and Safeguards

High-resolution alpha-particle spectrometry was performed with an ion-implanted silicon detector in vacuum on a homogeneously electrodeposited 236U 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.

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.

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.

The nuclide 231Pa is a member of the 235U decay chain. It is a complex alpha emitter with 25 identified alpha emissions. Formerly published alpha-particle emission probabilities were derived from measurements taken with magnetic spectrometers. This work presents the first measurements made with semiconductor detectors. High-resolution alpha-particle spectrometry was carried out at CIEMAT and JRC using ion-implanted planar silicon detectors. Alpha-particle emission probabilities of 23 transitions were derived from deconvolutions of the spectra. For the major lines, uncertainties are lower than 1%, a significant improvement to existing data. The new data set will allow a more accurate evaluation of the decay scheme of 231Pa.

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.

Two optical distance measurement devices have been compared for accurately defining the source-detector geometry of alpha-particle counters. The first consists of a travelling microscope with unifocal lens, to which a linear distance gauge is attached. The focusing is done by human eye. The second is a modern 3D coordinate measurement machine, equipped with a CMOS colour camera as the sensor. Focusing is performed automatically by software. With both devices, distance measurements of various drop-deposited sources on glass and stainless steel disks have been performed. There is a good mutual agreement of results. Even though the new device can sample more reference points, the accuracy of the measurements has not improved drastically due to the imperfect flatness of the sources. The main advantages of the new system are its ease of use and the lower health risk involved due to the larger distance between the performer and the source.

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.

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-2 π geometry. From these measurements, a new half-life value of T 1/2 ( 213 Bi)=45.62 (6) min was derived. Additionally, high-resolution alpha-spectrometry measurements were performed at a solid angle of 0.4% of 4π sr, 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 E α,0 =5878 (4) keV and E α,1 =5560 (4) keV were about 10 keV higher than validated data. The relative α-particle emission probabilities of 213 Bi, P α,0 =0.9155 (11) and P α,1 =0.0845 (11), and the 213 Bi alpha branching factor, P α =1− P β =2.140 (10)%, are compatible with recommended values, but have a higher accuracy.

International audience; 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 Earth's orbital distance to the sun could not be observed within 10(-5)-10(-6) range precision.

International audience; 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 Earth's 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.

High-resolution alpha-particle spectrometry was performed to determine the main alpha-particle emission probabilities in the decay of

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+β 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.

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.

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-2 π 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 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.

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; 4 πα + β 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-2 π 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 20.8 d 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.

International audience; 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.

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.

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.

In this paper the source preparation procedures for high-resolution 238U sources are described and compared. This work was done within collaboration between CIEMAT and IRMM in the frame of MetroFission, a project of the European Metrology Research Programme, in order to determine the alpha-emission probabilities of 238U. 238U was deposited from organic (iso-propanol) and inorganic-H2SO4/(NH4)2SO4, saturated NH4NO3-electrolyte solutions on metal backings. The parameters affecting electrodeposition were studied and optimized. The activity distribution of uranium was checked by autoradiography. Results show that the 238U source quality is significantly better using the saturated NH4NO3 than the two other electrolytes. By this method, sources of 18.6–22 mm diameter, 26 lg cm-2 surface density, *15–18 keV resolution and a peak to valley ratio higher than 50 could be made. This reconciles the inherently opposing requirements of high resolution and sufficient count rate needed to determine the alpha–emission probabilities accurately., JRC.D.4-Standards for Nuclear Safety, Security and Safeguards