Measurements of the absolute gamma-ray emission intensities from the decay of 166Ho.

166Ho (T1/2≈ 26.8 h) is an emerging theragnostic radionuclide of interest in nuclear medicine due to its peculiar decay scheme, featuring high-energy ß- emission (≈ 1.8 MeV) coupled with the main gamma-ray emission (≈ 80.6 keV). Using the new 166Ho activity standard and the well-calibrated, high-energy resolution HPGe detector, both available at ENEA-INMRI, a new determination of several 166Ho gamma-ray emission intensities, Iγ, was performed with low uncertainty. The new Iγ values contributed to the Decay Data Evaluation Project.

Seasonal variation of background counting rates in liquid scintillation counting.

A liquid scintillation background sample was measured daily in a custom-built TDCR counter for more than 17 months. The double and triple coincidence counting rates exhibit an annual sinusoidal fluctuation with a maximum in winter and a minimum in summer. Possible correlations with air temperature, air humidity, radon concentration and secondary cosmic radiation were investigated. The observation of a correlation with the ambient dose equivalent rate [Formula: see text] originating from the charged component of secondary cosmic radiation and an anti-correlation with the effective atmospheric temperature Teff suggest that the seasonal fluctuations in the background counting rate may be primarily driven by temporal variations in the muon flux at ground level. Additionally, a correlation was found with the indoor 222Rn concentration in air.

Liquid scintillation efficiencies, gamma-ray emission intensities, and half-life for Gd-153.

Gadolinium-153 was standardized for activity by live-timed anticoincidence counting and an ampoule was submitted to the international reference system (SIR). Absolute emission intensities for the main γ rays were determined with calibrated high-purity germanium (HPGe) and lithium-drifted silicon (Si(Li)) detectors. A revised decay scheme is indicated, with no probability of direct electron capture to the 153Eu ground state. Triple-to-double coincidence ratio (TDCR) efficiency curves indicate that the revised decay scheme is consistent with experiment. Half-life measurements agree with a previous NIST determination and show no sensitivity to chemical environment.

Estimation of gross α-ß and tritium activities in groundwater samples using LSC-TDCR technique in and around the geothermal region of Eastern India.

The present study is an attempt to assess the radiogenic quality of groundwater on the basis of gross α, gross ß and tritium (3H or H-3) activities in the Bakreswar-Tantloi geothermal region of Chotanagpur Plateau, West Bengal and Jharkhand, India. The aforesaid parameters in groundwater samples were measured using liquid scintillation counting triple to double coincidence ratio (LSC-TDCR) technique. Groundwater samples collected from Bakreswar-Tantloi geothermal region show gross α activities from below the minimum detectable activity (BMDA) to 0.5 ± 0.05 Bq/L, gross ß activities from BMDA to 0.2 ± 0.01 Bq/L and H-3 activities from BMDA to 63.42 Bq/L. The average gross α, gross ß and H-3 activities are also within the permissible limits prescribed by the World Health Organization (WHO). Though the annual effective doses in some samples were higher than the reference dose level of 0.1 mSv, the overall result suggests that the groundwater in the Bakreswar-Tantloi geothermal region is radiologically safe considering the radionuclides covered in this study.

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.

Uncertainties in TDCR measurement revisited: Contribution of optical effects.

In the Triple to Double Coincidence Ratio method in Liquid Scintillation Counting, the detection efficiency is calculated from the value of a free parameter describing the intrinsic light yield of the counting system. This model is generally based on a Poisson distribution of the number of photoelectrons detected and the detection efficiency is obtained from the complement of the non-detection efficiency. In the classical free parameter model, the mean of the Poisson distribution, m, is a constant but some variability of this mean could be expected from optical effects due to internal reflections inside the LS source or from non-homogeneity of the detection efficiency of the photomultiplier tubes. Then, m becomes a random variable and the distribution of the photoelectrons becomes a compound Poisson distribution, with a random variable as mean value. This paper explores the implications of the variance of m, which were, to our knowledge, never considered previously in the uncertainty budget of TDCR measurements.

Towards a radon-in-water primary standard at LNHB.

Despite widespread radon-in-water measurements, no primary radon-in-water standards currently exist. This work aims to bridge this gap by developing a system to produce radon-in-water reference materials. The system relies on cryogenic, loss-free transfer of radon, which is standardized through defined solid angle measurements, to a radon standard in water. It allows for preparation of liquid scintillation and gamma-ray spectrometry samples with traceable radon-in-water concentrations. The system's design, functionality, and the results of pilot performance tests are described.

Activity standardisation of 32Si at IRA-METAS.

This work explores the primary activity standardisation of 32Si as part of the SINCHRON project that aims at filling the geochronological dating gap by making a new precise measurement of the half-life of this nuclide. The stability of some of the radioactive test solutions, providing 32Si as hexafluorosilicic acid (H232SiF6), was monitored over long periods, pointing to the adequate sample composition and vial type to ensure stability. These solutions were standardised using liquid scintillation counting with the triple to double coincidence ratio (TDCR) technique and the CIEMAT-NIST efficiency tracing (CNET) method. Complementary backup measurements, using 4πß-γ coincidence counting with 60Co as a tracer, were performed with both liquid and plastic scintillation for beta detection. While 60Co coincidence tracing with a liquid scintillator predicted activities in agreement with the TDCR and CNET determinations, using plastic scintillation turned out to be unfeasible as the addition of lanthanum nitrate and ammonia to fix the silicon during the drying process generated large crystals that compromised the linearity of the efficiency function.

Activity standardization of 60Co and 106Ru/106Rh by means of the TDCR method and the importance of the beta spectrum.

Atomic and nuclear data represent an important input for the accuracy of primary activity measurements based on liquid scintillation. In particular, the reliability of ß-spectrum computation has been investigated for several years through experimental and theoretical studies providing solid evidence for the need to consider the atomic effects. In the present study, the activity standardization of two ß-emitting radionuclides (60Co, 106Ru/106Rh) was carried out by means of the 4πß-γ coincidence and Triple-to-Double Coincidence Ratio (TDCR) methods. The comparison between the activity concentrations given by both primary techniques presents new evidence that a better agreement is obtained when the exchange and screening effects are included in the ß-spectra implemented in the model of light emission for TDCR measurements. A new development of a stochastic model based on Geant4 simulations for TDCR calculations is also presented.

Activity standardisation of 177Lu.

177Lu decays through low-energy ß-- and γ-emissions in addition to conversion and Auger electrons. To support the use of this radiopharmaceutical in Switzerland, a 177Lu solution was standardised using the ß-γ coincidence technique, as well as the TDCR method. The solution had no 177mLu impurity. Primary coincidence measurements, with plastic scintillators for beta detection, were carried out using both analogue and digital electronics. TDCR measurements using only defocusing were also made. Monte Carlo calculations were used to compute the detection efficiency. The coincidence measurements with both analogue and digital electronics are compatible within one standard uncertainty, but they are lower than (and discrepant with) the TDCR measurements. An ampoule of this solution was submitted to the BIPM as a contribution to the Système International de Référence.

A bilateral comparison between LNHB and PTB to determine the activity concentration of the same 125I solution.

A bilateral comparison to determine the activity concentration of the same 125I solution was organized. As electron-capture radionuclide with a rather high atomic number, 125I 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 125I. 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.

Activity determination of 56Mn using extended TDCR-Cerenkov method.

The accuracy of activity determination for activated nuclide 56Mn is the key to the manganese bath method applying to the characterization of radionuclide neutron source. As an alternative to the 4π(C)-γ method, TDCR-Cerenkov method could also be applied to the measurement of 56Mn in the manganese bath device, if the existing calculation model is extended. There are two difficulties when the existing TDCR-Cerenkov method is applied to the activity determination of 56Mn. One is that the efficiency computation of gamma transitions, and the other is the interference contributed by Cerenkov photons emitted in the photomultiplier windows induced by Compton scattering. In this study, the above two difficulties are solved by extending the calculation model. For efficiency computation, the decay scheme of 56Mn is taken into account in the calculation of efficiency. Among them, the efficiency of gamma transition is calculated from the simulated secondary electronic spectra. In addition, Cerenkov photons emitted in photomultiplier windows are corrected by additional light proof experiment and improved calculation model. The results derived from this extended method are in good agreement with other standardization technique.

Primary standardization of 212Pb activity by liquid scintillation counting.

An activity standard for 212Pb in equilibrium with its progeny was realized, based on triple-to-double coincidence ratio (TDCR) liquid scintillation (LS) counting. A Monte Carlo-based approach to estimating uncertainties due to nuclear decay data (branching ratios, beta endpoint energies, γ-ray energies, and conversion coefficients for 212Pb and 208Tl) led to combined standard uncertainties ≤ 0.20 %. Confirmatory primary measurements were made by LS efficiency tracing with tritium and 4παß(LS)-γ(NaI(Tl)) anticoincidence counting. The standard is discussed in relation to current approaches to 212Pb activity calibration. In particular, potential biases encountered when using inappropriate radionuclide calibrator settings are discussed.

Development of 4πß(LS)-γ digital coincidence counting system at NIM.

A new 4πß(LS)-γ digital coincidence counting (DCC) system has been developed at NIM. The system equipped with a triple-to-double coincidence ratio (TDCR) counter in the ß-channel and a NaI(Tl) scintillation detector in the γ-channel. A dedicated DCC software was designed for off-line implementation of 4πß(LS)-γ coincidence counting method. The software consists of three modules: software-based circuits module, dead-time and resolving-time correction module and efficiency extrapolation module, respectively. The performance of the newly developed 4πß(LS)-γ DCC system was demonstrated by a comparison measurement of Co-60 solution with the conventional 4πß(PC)-γ DCC system.

Activity standardization of two enriched 40K solutions for the determination of decay scheme parameters and the half-life.

In this paper we describe experiments on two enriched 40K solutions to accurately determine decay data. The first solution was measured in 2004/2005 by means of a gamma-ray spectrometer with low background and a liquid scintillation (LS) counter to apply the CIEMAT/NIST efficiency tracing method. A combination of results yields an emission probability of the 1461 keV gamma-rays of Pγ = 0.1030(11) which is lower than current results of data evaluations. The activity concentration of the second solution was also determined by means of LS counting, but here, the CIEMAT/NIST efficiency tracing method as well as the TDCR method were applied. Again, the result was combined with that of independent gamma-ray spectrometry and the gamma-ray emission probability was found to be Pγ = 0.1029(9) in good agreement with the result obtained from the first solution. A combination of both experiments yields Pγ = 0.1029(9). The spectra of a TriCarb LS counter were carefully analyzed and a beta minus emission probability [Formula: see text]  = 0.8954(14) was determined. The new results for Pγ and [Formula: see text] indicate that the overall probability of the decay via EC in recent data evaluations is overestimated. The LS counting efficiencies were computed with a stochastic model and up-to-date calculations of the beta spectrum and fractional EC probabilities were used. The final activity result of the second solution is combined with the outcome of a comprehensive isotopic analysis to determine the half-life of 40K which is found to be 1.2536(27) ·109 years. All above-stated uncertainties are standard uncertainties (k = 1).

Development of a portable TDCR system at NIM, China.

In order to meet the demand of on-site measurement for radionuclides, a portable liquid scintillation TDCR system was developed at National Institute of Metrology (NIM), China. The system consists small size TDCR counter for the measurement of liquid scintillation sources, and digital electronics for pulse signal processing. The optical chamber adopts Teflon material with high diffuse reflection efficiency. Two independent signal processing solutions were used here for TDCR counting. One employed the on-line TDCR solution based on FPGA counting module named TDCR-DMCA, and the other adopted the off-line TDCR solution based on a stand-alone desktop digitizer of CAEN. Two solutions are applied to perform coincidence, dead-time and counting operations follow by MAC3 logic. The performance of the TDCR counting system was tested in benchmark comparison with the traditional custom-built TDCR counting system at NIM through activity measurements of 3H, 14C. Good agreement between these two systems was observed.

Simultaneous determination of actinides and 90Sr in large-size soil and sediment samples.

A simultaneous analytical method for sequential separation and determination of actinides and 90Sr in large-size environmental samples has been developed. In this method, successive co-precipitation steps were firstly conducted to remove matrix elements, then sequential column separation method was applied for simultaneous separation and purification of actinides and 90Sr/90Y. By using vacuum box technology, the total analytical time was minimized and batch processing allowed analyzing 12 samples in four days. The activity of 90Sr was obtained immediately by measuring its daughter radionuclide (90Y) with triple-to-double coincidence ratio (TDCR) Cherenkov counting, while the concentrations of Pu isotopes and 241Am could be measured by alpha spectrometry and mass spectrometric techniques. The overall recoveries of Pu, Am, Sr and Y were higher than 70% for the entire procedure, while the recovery ratios of Sr/Y were between 0.95 and 1.04 before chromatographic separation. The developed method was verified using 20 g and 50 g of environmental soil samples spiked with certified reference materials IAEA-384 or IAEA-385 and standard solution of 90Sr/90Y, and good agreement between the expected values and measured results has been achieved.

Activity standardisation of 223Ra.

We report here on the primary activity standardisation of a223Ra dichloride solution in equilibrium with its decay daughters. Both the triple-to-double-coincidence-ratio (TDCR) method with an in-house TDCR detector and the CIEMAT-NIST efficiency tracing (CNET) technique with a commercial counter were used. The liquid scintillation efficiencies for both methods are about 6 while the activities they predict with about 0.4% relative standard uncertainty agree within 0.15%. For backup, the solution was also standardised with 4πγ NaI(Tl) integral counting with a well-type NaI(Tl) detector, and efficiencies computed by Monte Carlo simulations using the GEANT code. This simple technique, unused previously for this nuclide, yielded an activity concentration compatible with, but 1% lower than, the one determined by liquid scintillation counting.

Ra-224 activity, half-life, and 241 keV gamma ray absolute emission intensity: A NIST-NPL bilateral comparison.

The national metrology institutes for the United Kingdom (UK) and the United States of America (USA) have compared activity standards for 224Ra, an α-particle emitter of interest as the basis for therapeutic radiopharmaceuticals. Solutions of 224RaCl2 were assayed by absolute methods, including digital coincidence counting and triple-to-double coincidence ratio liquid scintillation counting. Ionization chamber and high-purity germanium (HPGe) γ-ray spectrometry calibrations were compared; further, a solution was shipped between laboratories for a direct comparison by HPGe spectrometry. New determinations of the absolute emission intensity for the 241 keV γ ray (Iγ = 4.011(16) per 100 disintegrations of 224Ra) and of the 224Ra half-life (T1/2 = 3.6313(14) d) are presented and discussed in the context of previous measurements and evaluations.

Measurement of the absolute gamma-ray emission intensities from the decay of 103Pd.

Palladium-103 decays through electron capture to excited levels of 103Rh, and especially to the 39.748-keV metastable state. A high activity palladium chloride solution was standardized by liquid scintillation, using the Triple-to-Double Coincidence Ratio method. The absolute photon emission intensities were determined by gamma-ray spectrometry using point sources prepared with the standard solution. Different detectors and measuring conditions were used to cross-reference the results. The most intense photon emission intensities are derived with about 1% relative combined standard uncertainty.