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.

Measurement of the activity and determination of the half-life of 225Ac at POLATOM.

A method for absolute measurements of the 225Ac activity in equilibrium with its progeny was developed. Measurements were performed using the triple-to-double coincidence ratio (TDCR) method in two different TDCR counters. The activity concentration of an 225Ac solution was determined and the solution was sent to the SIR system for a comparison. The half-life of 225Ac was determined by one of the TDCR counters and found to be 9.9150(63) days.

On the interpretation of annual oscillations in 32Si and 36Cl decay rate measurements.

The 32Si decay rate measurement data of Alburger et al. obtained in 1982-1986 at Brookhaven National Laboratory have been presented repeatedly as evidence for solar neutrino-induced beta decay. The count rates show an annual sinusoidal oscillation of about 0.1% amplitude and maximum at February-March. Several authors have claimed that the annual oscillations could not be explained by environmental influences on the set-up, and they questioned the invariability of the decay constant. They hypothesised a correlation with changes in the solar neutrino flux due to annual variations in the Earth-Sun distance, in spite of an obvious mismatch in amplitude and phase. In this work, environmental conditions at the time of the experiment are presented. The 32Si decay rate measurements appear to be inversely correlated with the dew point in a nearby weather station. Susceptibility of the detection set-up to local temperature and humidity conditions is a likely cause of the observed instabilities in the measured decay rates. Similar conclusions apply to 36Cl decay rates measured at Ohio State University in 2005-2012.

First direct determination of the 93Mo half-life.

This work presents the first direct measurement of the 93Mo half-life. The measurement is a combination of high-resolution mass spectrometry for the determination of the 93Mo concentration and liquid scintillation counting for determining the specific activity. A 93Mo sample of high purity was obtained from proton irradiated niobium by chemical separation of molybdenum with a decontamination factor larger than 1.6 × 1014 with respect to Nb. The half-life of 93Mo was deduced to be 4839(63) years, which is more than 20% longer than the currently adopted value, whereas the relative uncertainty could be reduced by a factor of 15. The probability that the 93Mo decays to the metastable state 93mNb was determined to be 95.7(16)%. This value is a factor of 8 more precise than previous estimations. Due to the man-made production of 93Mo in nuclear facilities, the result leads to significantly increased precision for modelling the low-level nuclear waste composition. The presented work demonstrates the importance of chemical separations in combination with state-of-the-art analysis techniques, which are inevitable for precise and accurate determinations of nuclear decay data.

Comparison of digital coincidence modules used at POLATOM and PTB for TDCR and 4πß(LS)-γ coincidence counters.

Activity measurements of 3H, 241Am and 60Co solutions were performed to compare digital coincidence modules used at PTB and POLATOM for TDCR and 4πß(LS)-γ coincidence counting. The activities determined with various coincidence modules connected in parallel to the same counter at PTB were found to be consistent. Observed discrepancies caused by differences in the coincidence resolving time did not exceed 0.14%. Accidental coincidences simulated by a frequency generator were registered, and the coincidence resolving time was determined.

Beta spectrometry with metallic magnetic calorimeters in the framework of the European EMPIR project MetroBeta.

The aim of the European Metrology Research Project MetroBeta is to improve the knowledge of the shapes of beta spectra, both in terms of theoretical calculation and measurement. The precise knowledge of beta spectra is required for the activity standardisation of pure beta emitters. Metallic magnetic calorimeters (MMCs), a type of cryogenic detectors, with the beta emitter embedded in the absorber have proven to be among the best beta spectrometers, in particular for low-energy beta transitions. Within this project, new designs of MMCs optimized for five different beta energy ranges were developed and a new detector module was constructed. The beta spectra of 151Sm, 14C and 99Tc have been measured so far; additional measurements with 36Cl are under preparation. Improved theoretical calculation methods and complementary measurement techniques complete the project.

Activity standardization of (22)Na.

The activity of a (22)Na solution was measured by means of two 4pibeta-gamma coincidence-counting techniques. The first method corresponds to the classical 4pibeta-gamma coincidence counting and requires the beta(+)-branching ratio. The second procedure is based on a variation of the distance between source and gamma detector. The efficiency for detecting the sum peak is then extrapolated to zero, giving the total source activity. The combination of both methods yields the beta(+) branching ratio. In addition, liquid scintillation counting using the CIEMAT/NIST-method as well as a secondary standardization by means of calibrated ionization chambers were used for activity determination. The results were checked for consistency and an ampoule was submitted to the BIPM to have the activity result entered into the database of the International Reference System (SIR).

Study of a Monte Carlo rearrangement model for the activity determination of electron-capture nuclides by means of liquid scintillation counting.

A new Monte Carlo approach for the computation of the electron spectra of electron-capture nuclides is applied to obtain efficiencies in liquid scintillation counting for CIEMAT/NIST applications. The new method is applied to the radionuclides (109)Cd and (125)I by using a stochastic atomic rearrangement model, taking into account rearrangement processes including L-, M-, and N-subshells. The counting efficiencies were computed with the new code MICELLE which also comprises an approach for calculating the counting efficiency of a radionuclide in a gel phase sample. The calculated counting efficiencies are compared with experimental results.

Calibration of a radionuclide calibrator system as a Bulgarian standard for activity.

A commercially available radionuclide calibrator of the type Curiementor 3 (PTW, Freiburg, Germany) was calibrated using activity standard solutions, from the Physikalisch-Technische Bundesanstalt (PTB), of a number of photon-emitting radionuclides, in particular those used in nuclear medicine: (18)F, (51)Cr, (67)Ga, (99m)Tc, (111)In, (123)I, (125)I, (131)I, (186)Re, (201)Tl, and for beta-emitting nuclides: (32)P, (89)Sr, (90)Y, (204)Tl. An energy-dependent efficiency curve was established to calculate efficiencies for photon-emitting radionuclides. The differences between experimental and calculated radionuclide efficiencies of the measuring system are of the order of a few percent. The performance of the system was checked for instrument stability, using a long-lived (137)Cs source, and for linearity using the decay of a (99m)Tc source. The calibration measurements were carried out with 2g of solution in standard PTB-type glass ampoules. The dependence of efficiency with varying solution mass and changing ampoule geometry is studied for some of the radionuclides. For example, geometry correction factors are determined for various solution volumes or ampoules with different wall thickness. The measuring system will enable the National Centre of Metrology (NCM) of Bulgaria to provide calibration services for activity measurements, which are traceable to PTB standards, and to organize national comparisons in order to improve the quality of measurements for nuclear medicine in Bulgarian hospitals. Furthermore, it should enable NCM to declare Calibration and Measurement Capabilities (CMCs) and to submit radioactive solutions to the International Reference System (SIR) at the BIPM in order to compare the results with Key Comparison Reference Values (KCRVs).

Determination of the shape factor of (90)Sr by means of the cutoff energy yield method.

Usually, Kurie plots are used to analyze beta-spectra shape-factor functions measured by means of semiconductor and magnetic spectrometers. A drawback of these techniques is the occurrence of self-absorption within the samples through which the emission spectrum is altered. In liquid-scintillation samples self-absorption does not occur, but the poor energy resolution makes the analysis of the spectra difficult. To overcome this problem, two resolution-invariant observables are used for determining the shape-factor function of (90)Sr: (1) the maximum point energy and (2) the cutoff energy yield. The measured shape-factor function of (90)Sr agrees with the one which is predicted by theory for the first-forbidden unique transition.

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.

Results of an international comparison of activity measurements of 68Ge.

An international key comparison, identifier CCRI(II)-K2.Ge-68, has been performed. The National Institute of Standards and Technology (NIST) served as the pilot laboratory, distributing aliquots of a 68Ge/68Ga solution. Results for the activity concentration, CA, of 68Ge at a reference date of 12h00 UTC 14 November 2014 were submitted by 17 laboratories, encompassing many variants of coincidence methods and liquid-scintillation counting methods. The first use of 4π(Cherenkov)ß-γ coincidence and anticoincidence methods in an international comparison is reported. One participant reported results by secondary methods only. Two results, both utilizing pure liquid-scintillation methods, were identified as outliers. Evaluation using the Power-Moderated Mean method results in a proposed Comparison Reference Value (CRV) of 621.7(11)kBqg-1, based on 14 results. The degrees of equivalence and their associated uncertainties are evaluated for each participant. Several participants submitted 3.6mL ampoules to the BIPM to link the comparison to the International Reference System (SIR) which may lead to the evaluation of a Key Comparison Reference Value and associated degrees of equivalence.

Comparison for quality assurance of (99m)Tc activity measurements with radionuclide calibrators.

In 2005, the Physikalisch-Technische Bundesanstalt (PTB) and the QSA Global GmbH (QSA) organised a national comparison of (99m)Tc solution measurements. The purpose of this comparison was to gain information on the quality of routine activity measurements carried out in the field of nuclear medicine in Germany. In addition to this, an ampoule containing a calibrated (99m)Tc solution was sent from PTB to the Bureau International des Poids et Mesures (BIPM) to have the activity result entered into the database of the International Reference System (SIR), and thus demonstrating traceability of the measurements to the SI. In the following, we will report on the activity standardisation carried out at the PTB, and on the way in which the national comparison had been organised, and we will provide information on the analysis as well as on its results.

Activity standardisation of (18)F and ionisation chamber calibration for nuclear medicine.

Primary activity standardisations were performed on solutions of (18)F using 4pibeta-gamma coincidence counting and liquid scintillation counting (LSC) according to the CIEMAT/NIST method. A beta(+)-emission probability of 96.86% was used for both methods. The various standardised (18)F solutions were measured in ionisation chambers of the Physikalisch-Technische Bundesanstalt (PTB) and compared by determining radionuclide calibration factors. Already in 2001 an (18)F solution had been standardised at the PTB and compared with the results of nine national metrology institutes (NMIs), using the ISOCAL IV secondary radionuclide calibrators of the National Physical Laboratory (NPL) as transfer instruments and a (68)Ge check source solution. These results were linked to the International Reference System (SIR) at the Bureau International des Poids et Mesures (BIPM) by aliquots of solutions sent by the Laboratoire National Henri Becquerel (BNM-LNHB) and the NPL. Further on, in 2005, PTB sent an aliquot of an (18)F solution to the SIR for ionisation chamber measurements. A value of the equivalent activity was determined and included in the key comparison database (KCDB). The recent PTB value of the equivalent activity of the SIR is in good agreement with the key comparison reference value determined from five NMIs. These results confirm that the standardisation of (18)F solutions can be achieved with the accuracy required for use in nuclear medicine and, in particular, for applications in positron emission tomography (PET).

A new method for secondary standard measurements with the aid of liquid scintillation counting.

A new secondary standard measuring procedure based on liquid scintillation counting has been developed at PTB. In this procedure, the efficiency curve, i.e. the counting efficiency of the nuclide to be investigated as a function of the tritium counting efficiency, is-in contrast to the CIEMAT/NIST method-not calculated but determined by experiment. For the measurements, gamma-emitting activity standards are used which were calibrated by other methods. The procedure was successfully used to calibrate solutions of the radionuclides 54Mn, 57Co, 65Zn, 85Sr and 125I with small uncertainties.

The LSC efficiency for low-Z electron-capture nuclides.

In this paper, we apply the CIEMAT/NIST method to the three low-Z electron-capture nuclides 54Mn, 55Fe and 65Zn by using the KLM and KL1L2L3M atomic rearrangement models, respectively. The counting efficiencies are computed with the new code EMILIA, which comprises an improved model for the interaction of low-energy X-rays with the scintillation cocktail. The calculated counting efficiencies are compared with experimental results.

Standardization and nuclear decay data of 65Zn.

Standardization by means of 4pibeta-gamma coincidence counting was applied to calibrate a 65Zn solution within the scope of EUROMET project no. 721. The activity result was combined with gamma-ray spectrometry measurements to investigate the photon emission probabilities. The half-life of 65Zn was measured with improved accuracy by means of 4pi ionization chamber measuring systems that were also used for secondary activity determination. In addition, we tested a new secondary standardization procedure by means of liquid scintillation counting.

Activity standardization and nuclear decay data of 109Cd.

The activity of a (109)Cd solution has been accurately determined without using (109)Cd nuclear decay data such as emission probabilities. An ampoule containing this calibrated (109)Cd solution was sent to the Bureau International des Poids et Mesures to include the activity result in the database of the International Reference System (SIR). The emission rate of conversion electrons was measured by means of pressurized proportional counters as well as by a liquid scintillation spectrometer. The combination of the results with the photon emission rate measured with the aid of gamma-ray spectrometers yields the activity concentration. The measurement results were also used to deduce emission probabilities with high accuracy. For the 88 keV transition, a photon emission probability of p(gamma)=0.03663(33) and a total internal conversion coefficient of alpha(t)=26.30(25) were determined.

Comparison of calculated spectra for the interaction of photons in a liquid scintillator. Example of 54Mn 835 keV emission.

The CIEMAT/NIST and TDCR methods in liquid scintillation counting, initially developed for the activity standardization of pure-beta radionuclides, have been extended to the standardization of electron capture and beta-gamma radionuclides. Both methods require the calculation of the energy spectrum absorbed by the liquid scintillator. For radionuclides emitting X-rays or gamma-rays, when the energy is greater than a few tens of keV the Compton interaction is important and the absorption is not total. In this case, the spectrum absorbed by the scintillator must be calculated using analytical or stochastic models. An illustration of this problem is the standardization of 54Mn, which is a radionuclide decaying by electron capture. The gamma transition, very weakly converted, leads to the emission of an 835 keV photon. The calculation of the detection efficiency of this radionuclide requires the calculation of the energy spectrum transferred to the scintillator after the absorption of the gamma ray and the associated probability of absorption. The validity of the method is thus dependent on the correct calculation of the energy transferred to the scintillator. In order to compare the calculation results obtained using various calculation tools, and to provide the metrology community with some information on the choice of these tools, the LS working group of the ICRM organised a comparison of the calculated absorbed spectra for the 835 keV photon of 54Mn. The result is the spectrum of the energy absorbed by the scintillator per emission of an 835 keV gamma ray. This exercise was proposed for a standard 20 ml LS glass vial and for LS cocktail volumes of 10 and 15 ml. The calculation was done for two different cocktails: toluene and a widely used commercial cocktail, Ultima Gold. The paper describes the results obtained by nine participants using a total of 12 calculation codes.

Half-life measurements of 87Rb by liquid scintillation counting.

The specific activity of natural 87Rb was measured by means of 4pibeta liquid scintillation counting in a two-photomultiplier-tube spectrometer. 3H-efficiency tracing was used together with the CIEMAT/NIST method to obtain the detection efficiency. For this purpose a new parameterization of the shape factor for the third forbidden non-unique beta-transition was performed. The hygroscopic behaviour of the salts used for sample preparation was studied. The half-life of 87Rb was found to be T1/2 = 4.967(32) x 10(10)y.