Search

An aqueous solution of 99m Tc was standardized by means of 4πce(LS)-γ and 4πce(PC)-γ coincidence counting. The activity concentration was obtained by efficiency extrapolation relying on four different variation techniques. In both setups, fast digitizers were used for data acquisition. Detected events were recorded in list mode format, and their coincidence relationship was analyzed in the subsequent offline analysis. The combined result was used to participate in an international comparison using the Transfer Instrument of the International Reference System., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

A bilateral comparison to determine the activity concentration of the same 125 I solution was organized. As electron-capture radionuclide with a rather high atomic number, 125 I must be regarded as difficult to measure. The situation is partly exacerbated by the fact that some established standardization methods, like photon-photon coincidence counting, can no longer be applied due to the unavailability of appropriate equipment and expertise. One aim of this work is to compare modern liquid scintillation counting methods for the standardization of 125 I. Both participating metrology institutes have used their custom-built triple-to-double-coincidence ratio (TDCR) counters and the determined activity concentrations are in excellent agreement even though the ways to analyze the data and to compute counting efficiencies were widely independent. The results also agree with the outcome of 4π-γ counting that was carried out at LNHB. In both laboratories, the measurements were complemented by measurements with several secondary standardization methods which even allow to establish a link to the CCRI(II)-K2.I-125(2) comparison started in 2004. A good agreement between the TDCR results and the key comparison reference value of the 2004/2005 comparison was obtained., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

The Bureau International des Poids et Mesures (BIPM) is developing a new transfer instrument to extend its centralized services for assessing the international equivalence of radioactive standards to new radionuclides. A liquid scintillation counter using the triple/double coincidence ratio method is being studied and tested in the CCRI(II)-P1.Co-60 pilot study. The pilot study, involving 13 participating laboratories with primary calibration capabilities, validated the approach against the original international reference system based on ionization chambers, which has been in operation since 1976. The results are in agreement and an accuracy suitable for purpose, below 5×10 -4 , is achieved. The pilot study also reveals an issue when impurities emitting low-energy electrons are present in the standard solution, which have a different impact on liquid scintillation counting compared to other primary measurement methods., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Activity measurements of 3 H, 241 Am and 60 Co solutions were performed to compare digital coincidence modules used at PTB and POLATOM for TDCR and 4πβ(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., (Copyright © 2020 The Authors. Published by Elsevier Ltd.. All rights reserved.)

The activity concentration of an 225 Ac solution was determined by means of liquid scintillation counting using three custom-built TDCR counters. The efficiency calculation was carried out in the same way as it had been done in an earlier article on 229 Th. The computation of the counting efficiency is rather complex and requires a correction to allow for the short-lived 213 Po. The experimental deadtime was varied to validate the correction. One of the TDCR counters is equipped with a CAEN N6751C digitizer for data acquisition. In addition, the system comprises a CeBr 3 solid scintillator as a gamma detector. The offline analysis was used to obtain a time-difference spectrum, using signals from the 213 Po γ-rays at about 440 keV in the gamma channel in coincidence with the preceding beta decay as the start signal, and signals from the subsequent (delayed) 213 Po alpha decays as the stop signal. After fitting an exponential function with a constant background, the half-life of 213 Po was determined to be 3.709(12) μs, which is in good agreement with the evaluated value. The half-life of 225 Ac was determined from long-term measurements using an ionization chamber (IC) and a TDCR system. The combined result was found to be 9.9179(30) d, which is in agreement with the outcome from Pommé et al. (2012)., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2019 The Authors. Published by Elsevier Ltd.. All rights reserved.)

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 151 Sm, 14 C and 99 Tc have been measured so far; additional measurements with 36 Cl are under preparation. Improved theoretical calculation methods and complementary measurement techniques complete the project., (Copyright © 2019 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Liquid scintillation samples with 227 Th were prepared a few hours after the separation of the progeny. During the measurements, 227 Th and its daughters are not in radioactive equilibrium. The counting efficiencies of the individual radionuclides of the decay chain differ from each other and the activity of an individual progeny relative to the activity of 227 Th varies with time. Hence, the overall counting efficiency varies with time as well. The counting efficiency ε T227h++ of 227 Th and its progeny was determined by means of the CIEMAT/NIST efficiency tracing method. The free parameter is derived from the quench-indicating parameter, SQP(E), and from 3 H tracer measurements. This makes it possible to compute the efficiency ε T227h++ as a function of time. The individual efficiencies of all progeny are to be combined, taking correction factors and activity ratios into account. Thereby, a new, time-dependent correction, namely for the decay during the measurements, is applied. With this method, activity results are obtained that are stable over a long period of time. A least-squares method yields the time of the chemical separation as well as the 227 Th half-life, which was also obtained by means of measurements in an ionization chamber. The weighted mean of the two methods (CIEMAT/NIST efficiency tracing and measurements in ionization chambers) was found to be T 1/2 = 18.681(9) d., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

The radionuclide 129 I is a long-lived fission product that decays to 129 Xe by beta-particle emission. It is an important tracer in geological and biological processes and is considered one of the most important radionuclides to be assessed in studies of global circulation. It is also one of the major contributors to radiation dose from nuclear waste in a deep geological repository. Its half-life has been obtained by a combination of activity and mass concentration measurements in the frame of a cooperation of 6 European metrology institutes. The value obtained for the half-life of 129 I is 16.14 (12) × 10 6 a, in good agreement with recommended data but with a significant improvement in the uncertainty., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

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, β - , β + 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., (Copyright © 2017 The Authors. Published by Elsevier Ltd.. All rights reserved.)

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 68 Ge/ 68 Ga solution. Results for the activity concentration, C A , of 68 Ge 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)β-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., (Published by Elsevier Ltd.)

The activity of a 67 Ga solution was measured by means of the 4πβ-γ coincidence counting technique. A setup with a proportional counter and non-extending dead-time modules in the two detector channels was used. The influence of the delayed state affecting the measured count rates was taken into account by using appropriate correction formulae. The analysis requires a variation of the dead time and a subsequent extrapolation to infinite dead time. An uncertainty of about 0.5% was obtained and the result was used to make an intercomparison with the SIR of the BIPM., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

A commercially available Fidelis ionization chamber was calibrated and assessed in PTB with activity standard solutions. The long-term stability and linearity of the system was checked. Energy-dependent efficiency curves for photons and beta particles were determined, using an iterative method in Excel™, to enable calibration factors to be calculated for radionuclides which were not used in the calibration. Relative deviations between experimental and calculated radionuclide efficiencies are of the order of 1% for most photon emitters and below 5% for pure beta emitters. The system will enable TAEK-SANAEM to provide traceable activity measurements., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

In 2014, PTB and the company Eckert & Ziegler organized a national comparison exercise to determine the activity of a (90)Y solution. One aim of the comparison was to assess the measurement capability of hospitals and medical practices in Germany. P6-type vials were filled with aliquots of a radioactive (90)Y solution and then sent to 19 participants who were asked to measure the activity in the ampoules as well as in their own standard geometry using syringes. Most of the submitted results have a deviation of less than ±10% from the PTB reference activity when measured in the P6-type vials. The spread is somewhat larger when measured in a syringe geometry. The comparison revealed that some participants have difficulties in applying decay corrections and only a few participants were capable of estimating realistic measurement uncertainties., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

The activity concentrations of solutions containing 227 Ac and 223 Ra in equilibrium with their progenies, respectively, were measured by means of liquid scintillation counting. The counting efficiencies were determined with the aid of a free parameter model. The corresponding calculations comprise the computation of several alpha, beta and beta/gamma branches. For short-lived progenies like 215 Po the counting efficiency depends on the counter dead time. Measurements were made in custom-built triple-to-double coincidence ratio (TDCR) systems and various dead-time adjustments were used. In addition, two commercial counters were used to apply the CIEMAT/NIST efficiency tracing technique using 3 H as a tracer. For the 227 Ac solution, the overall relative standard uncertainty of the activity concentration was found to be 0.93%. The dominant uncertainty components are assigned to the efficiency computation of the low-energy beta transitions of 227 Ac. We have identified a need for improved 227 Ac decay data to achieve a significant reduction in the overall uncertainty. In the case of 223 Ra, the activity concentrations were determined with relative standard uncertainties below 0.3%. Hence, PTB is prepared to provide calibration services for 223 Ra, which is an isotope of increasing interest in nuclear medicine. The TDCR measurements were also used to determine the half-life of 223 Ra. The decay was followed for about 58 days and a half-life T 1/2 =11.4362(50)d was obtained., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

The triple-to-double-coincidence ratio method (TDCR) is an important method for activity standardization in metrology institutes worldwide. There is an increasing interest in portable systems that allow activity determination outside of specialized laboratories with high accuracy. Within the framework of the EMRP "MetroFission" project, several portable systems using different designs were developed. The PTB system described here is based on channel photomultipliers incorporated in a portable detection module, a separate electronics bin and a computer for data acquisition and storage. This miniature TDCR system was extensively tested and compared to the PTB reference TDCR system that is very well characterized and has been used in several intercomparisons., (© 2013 Published by Elsevier Ltd.)

The triple-to-double coincidence ratio (TDCR) method is frequently used to measure the activity of radionuclides decaying by pure β emission or electron capture (EC). Some radionuclides with more complex decays have also been studied, but accurate calculations of decay branches which are accompanied by many coincident γ transitions have not yet been investigated. This paper describes recent extensions of the model to make efficiency computations for more complex decay schemes possible. In particular, the MICELLE2 program that applies a stochastic approach of the free parameter model was extended. With an improved code, efficiencies for β(-), β(+) and EC branches with up to seven coincident γ transitions can be calculated. Moreover, a new parametrization for the computation of electron stopping powers has been implemented to compute the ionization quenching function of 10 commercial scintillation cocktails. In order to demonstrate the capabilities of the TDCR method, the following radionuclides are discussed: (166m)Ho (complex β(-)/γ), (59)Fe (complex β(-)/γ), (64)Cu (β(-), β(+), EC and EC/γ) and (229)Th in equilibrium with its progenies (decay chain with many α, β and complex β(-)/γ transitions)., (© 2013 Published by Elsevier Ltd.)

Liquid scintillation measurements of (229)Th in radioactive equilibrium with its progenies were carried out. The counting efficiency was determined by means of a free parameter model. The measurements were made in a custom-built triple-to-double coincidence ratio (TDCR) system. In addition, a new portable mini-TDCR system with three channel photomultipliers and two commercial counters were tested. The decay of the short-lived (213)Po requires great care, since it often occurs during the dead time of the counter systems. Also the rather short-lived (217)At may decay during the dead time caused by (221)Fr decay events. The overall counting efficiency of the TDCR system of PTB was found to be about 700% (depending on the degree of chemical quenching) and the relative standard uncertainty of the activity concentration was found to be about 0.23%. The determined activity concentration was compared with the outcome of alpha spectrometry under defined solid angle and excellent agreement was found. The TDCR efficiency calculations can be easily adapted to activity determinations of (225)Ra or (225)Ac in equilibrium with their progenies., (© 2013 Published by Elsevier Ltd.)

In the past few years, two Čerenkov methods were developed to make activity measurements of high-energy beta emitters in liquid scintillation counters with two or three photomultiplier tubes (PMTs) possible. Both methods are based on a free parameter model and make use of the Frank and Tamm theory for the emission of Čerenkov light. In this article, additional effects are discussed and further improvements are presented. The dependence of the refractive index of water on the wavelength can now be taken into account, which has also an influence on the upper limit of the wavelength region for the production of Čerenkov light. In addition, the dependence of the PMT response on the wavelength is taken into account. Finally, it is possible to take a potential asymmetry of efficiencies in a system with three PMTs into account. To this end, three free parameters are assigned to each individual PMT and then determined by means of a downhill simplex optimization algorithm. The computed counting efficiencies for a triple-to-double coincidence ratio (TDCR) system were compared with experimental data for (32)P, (89)Sr, and (90)Y., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

The purposes of this study were to create national activity standards of (64)Cu, to make possible the definition of an international key comparison reference value and to determine the decay data in order to improve the decay scheme. Four laboratories measured the activity of a (64)Cu solution; these results were compared through the International Reference System. Moreover, the laboratories carried out new measurements of the photon emission intensities and of the half-life. A new decay scheme was derived from these new values and the previously published ones., (Copyright © 2012 Elsevier Ltd. All rights reserved.)

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., (Copyright © 2012. Published by Elsevier Ltd.)

A procedure has been developed to calibrate photon-emitting wide area reference sources in terms of activity, surface emission rate and uniformity considering the requirements introduced by the recent revision of ISO standard 8769. The method makes use of a large volume NaI detector with a cross table scanning system, a radiography system and it applies Monte Carlo techniques to assess the surface emission rate. The method was successfully applied to sources of (241)Am, (57)Co, (137)Cs and (60)Co. In addition, problems with definitions and the practical use of standard ISO 8769:2010 are highlighted., (Copyright © 2012 Elsevier Ltd. All rights reserved.)

The radionuclide (113m)Cd was extracted from a Cd component, which has been irradiated in a research reactor during its routine operation. A validated separation procedure was then used to obtain a (113m)Cd solution of high radiochemical purity. The solution was measured by means of liquid scintillation counting for activity determination. To this end, the CIEMAT/NIST efficiency tracing method as well as the triple-to-double coincidence (TDCR) counting technique were used. Measurements in a low-background gamma-ray spectrometer were applied to identify any potential photon-emitting impurities and to measure the 263.7 keV photons from the isomer transition. A gamma emission probability of 0.01839(29)% was determined for this line. The liquid scintillation measurements were also used to evaluate the half-life of (113m)Cd. The decay was followed for about 11 months and a half-life T(1/2)=13.97(13) years was obtained., (Copyright © 2010 Elsevier Ltd. All rights reserved.)

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, six of which sent results for photon emission intensities both in absolute and in relative terms. From these results and including previous published values, a consistent decay scheme was worked out, proving that problems in activity measurements have not been due to decay scheme data., (Copyright 2010 Elsevier Ltd. All rights reserved.)

A triple-to-double coincidence ratio (TDCR) liquid scintillation counting system (Pochwalski et al., 1988; Grau Malonda and Coursey, 1988) was set up at the Physikalisch-Technische Bundesanstalt (PTB) to be used as an additional technique for primary activity standardization. The optical chamber of the system was designed in our laboratory, expending great effort to achieve maximum light transmission to the photomultiplier tubes (PMT) and, consequently, a maximum counting efficiency and low uncertainties. A programme to compute the counting efficiencies and to analyse the measurement data was developed and tested. The software can also be used to allow for PMT asymmetries. The system and recently developed analysis procedures were used for the activity standardization of a tritiated water solution within the scope of an international comparison under the auspices of the Bureau International des Poids et Mesures (BIPM)., (Copyright 2009 Elsevier Ltd. All rights reserved.)

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., (Copyright 2010 Elsevier Ltd. All rights reserved.)

The half-life of the long-lived isotope (147)Sm was determined by means of activity determination using liquid scintillation counting. The amount of samarium was determined by ICP-OES using a NIST reference standard. The isotopic ratio N((147)Sm)/N(Sm) of the samples was measured by means of ICP-HRMS. The half-life was found to be 1.070(9)x10(11) y. The result is in good agreement with other evaluations and the relative standard uncertainty of 0.8% is lower than in any previous work.

The sum-peak method was successfully applied to the determination of the activity of extended (60)Co sources measured on a HPGe detector. Monte Carlo simulations were used to account for the effects of the spatial variation of the efficiency across the sample volume and for the angular correlations between the emitted gamma rays. The determined activities agree with the reference values within a range of 1.0%.

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).