Determination of the Terbium-152 half-life from mass-separated samples from CERN-ISOLDE and assessment of the radionuclide purity.

Terbium-152 is one of four terbium radioisotopes that together form a potential theranostic toolbox for the personalised treatment of tumours. As 152 Tb decay by positron emission it can be utilised for diagnostics by positron emission tomography. For use in radiopharmaceuticals and for activity measurements by an activity calibrator a high radionuclide purity of the material and an accurate and precise knowledge of the half-life is required. Mass-separation and radiochemical purification provide a production route of high purity 152Tb. In the current work, two mass-separated samples from the CERN-ISOLDE facility have been assayed at the National Physical Laboratory to investigate the radionuclide purity. These samples have been used to perform four measurements of the half-life by three independent techniques: high-purity germanium gamma-ray spectrometry, ionisation chamber measurements and liquid scintillation counting. From the four measurement campaigns a half-life of 17.8784(95) h has been determined. The reported half-life shows a significant difference to the currently evaluated half-life (ζ-score = 3.77), with a relative difference of 2.2 % and an order of magnitude improvement in the precision. This work also shows that under controlled conditions the combination of mass-separation and radiochemical separation can provide high-purity 152Tb.

A plastic scintillator and HPGe ß-γ coincidence detection system.

A network of specialist laboratories support the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) with re-measurements of radionuclide samples, including xenon gas. The measurement of four xenon fission product radionuclides (133Xe, 135Xe, 131mXe and 133mXe) can be used to detect an underground nuclear explosion. Laboratories use a range of techniques to measure the radionuclides, including beta-gamma (ß-γ) coincidence spectrometry. These highly-sensitive measurements are capable of detecting concentrations of down to 500 atoms of 133Xe in a few cm3 of xenon. In some detector systems, detection of the metastable isomers (131mXe and 133mXe) can be more challenging due to interferences between the signatures of different radionuclides. Recent work has shown that using high-purity Germanium (HPGe) high-resolution gamma detectors, these interferences can be reduced, lowering the dependence of the detection limits on radionuclide sample isotopic composition. One downside of these detectors is the reduction in detection efficiency, which impacts the overall detection sensitivity; so assessing different detector systems is a priority for radionuclide laboratories. This work presents a coincidence detector system comprising of a plastic scintillator gas cell and a large-crystal high-purity germanium detector. The energy resolution, coincidence detection efficiency, MDA and interference factors are determined from measurements of synthetic radioxenon gas samples.

Half-life determination of 155Tb from mass-separated samples produced at CERN-MEDICIS.

Terbium-155 has been identified for its potential for single-photon emission computed tomography (SPECT) in nuclear medicine. For activity measurements, an accurate and precise half-life of this radionuclide is required. However, the currently evaluated half-life of 5.32(6) d with a relative standard uncertainty of 1.1% determines the precision possible. Limited literature for the half-life measurements of this radionuclide is available and all reported investigations are prior to 1970. Further measurements are therefore needed to confirm the accuracy and improve the precision of the half-life for its use in the clinical setting. Two samples produced and mass separated at the CERN-MEDICIS facility have been measured at the National Physical Laboratory by two independent techniques: liquid scintillation counting and high-purity germanium gamma-ray spectrometry. A half-life of 5.2346(36) d has been determined from the weighted mean of the half-lives determined by the two techniques. The half-life reported in this work has shown a relative difference of 1.6% to the currently evaluated half-life and has vastly improved the precision.

Determination of the 161Tb half-life.

There is significant interest in the use of terbium radioisotopes for applications in cancer therapy and diagnosis. Of these, 161Tb, as a medium energy beta-emitter, is being investigated as a potential alternative to 177Lu. The relatively high proportion of conversion electron and Auger electron emissions per decay make 161Tb an attractive targeted therapeutic. As a product of nuclear fission, 161Tb is also of importance to nuclear forensics. The standard uncertainty of the current evaluated half-life of 6.89(2) d contributes significantly to the standard uncertainty of any decay corrected activity determination made. Furthermore, the accuracy of this evaluated half-life has been called into question by measurements reported in 2020 at the Institute of Radiation Physics (IRA), Switzerland, who reported a half-life of 6.953(2) d. In the current work, the half-life of the 161Tb ground state decay has been measured at three independent laboratories located in the United Kingdom and the United States of America for a total of six determinations using three independent measurement techniques; gamma-ray spectrometry, ionisation chamber measurement and liquid scintillation counting. The half-life determined for 161Tb of 6.9637(29) d confirms the observed 1% relative increase observed by IRA, though the reported half-lives in this work and at IRA are significantly different (ζ-score = 3.1).

Competition between Allowed and First-Forbidden ß Decay: The Case of

The ß decay of ^{208}Hg into the one-proton hole, one neutron-particle _{81}^{208}Tl_{127} nucleus was investigated at CERN-ISOLDE. Shell-model calculations describe well the level scheme deduced, validating the proton-neutron interactions used, with implications for the whole of the N>126, Z<82 quadrant of neutron-rich nuclei. While both negative and positive parity states with spin 0 and 1 are expected within the Q_{ß} window, only three negative parity states are populated directly in the ß decay. The data provide a unique test of the competition between allowed Gamow-Teller and Fermi, and first-forbidden ß decays, essential for the understanding of the nucleosynthesis of heavy nuclei in the rapid neutron capture process. Furthermore, the observation of the parity changing 0^{+}→0^{-}ß decay where the daughter state is core excited is unique, and can provide information on mesonic corrections of effective operators.

Advances in the Direct Study of Carbon Burning in Massive Stars.

The ^{12}C+^{12}C fusion reaction plays a critical role in the evolution of massive stars and also strongly impacts various explosive astrophysical scenarios. The presence of resonances in this reaction at energies around and below the Coulomb barrier makes it impossible to carry out a simple extrapolation down to the Gamow window-the energy regime relevant to carbon burning in massive stars. The ^{12}C+^{12}C system forms a unique laboratory for challenging the contemporary picture of deep sub-barrier fusion (possible sub-barrier hindrance) and its interplay with nuclear structure (sub-barrier resonances). Here, we show that direct measurements of the ^{12}C+^{12}C fusion cross section may be made into the Gamow window using an advanced particle-gamma coincidence technique. The sensitivity of this technique effectively removes ambiguities in existing measurements made with gamma ray or charged-particle detection alone. The present cross-section data span over 8 orders of magnitude and support the fusion-hindrance model at deep sub-barrier energies.

The impact of high-energy tailing in high-purity germanium gamma-ray spectrometry on the activity determination of 224Ra using the 241.0 keV emission.

High-energy tailing is an often-overlooked component in high-purity germanium gamma-ray spectrometry when performing the non-linear least squares fit of a full-energy peak. This component comes from the incomplete restoration of the baseline prior to the next pulse being processed and therefore is an issue of increased count rates. In the current work, the impact of this oversight is shown through the dynamics and decay characteristics of 224Ra and its radioactive decay progeny. Multiple measurements of two samples, separated from the decay progeny and at differing activities, have been made. The results of full-energy peak fitting of the convoluted 238.6 keV and 241.0 keV full-energy peaks with and without the high energy tailing component are presented. Trends in the observed activity that approximate the ingrowth of 212Pb have been observed where no high-energy tailing component is used, with maximum relative differences of 2% and 5% determined.

Selective sorption of uranium from aqueous solution by graphene oxide-modified materials.

The effect of competing ions on the sorption behaviour of uranium onto carboxyl-functionalised graphene oxide (COOH-GO) were studied in batch experiments in comparison to graphene oxide (GO) and graphite. The effect of increasing the abundance of select chemical functional groups, such as carboxyl groups, on the selectivity of U sorption was investigated. In the course of the study, COOH-GO demonstrated superior performance as a sorbent material for the selective removal of uranyl ions from aqueous solution with a distribution coefficient of 3.72 ± 0.19 × 103 mL g-1 in comparison to 3.97 ± 0.5 × 102 and 2.68 ± 0.2 × 102 mL g-1 for GO and graphite, respectively.

Investigation of γ-γ coincidence counting using the National Nuclear Array (NANA) as a primary standard.

The National Physical Laboratory has recently been in the process of commissioning a multi-detector γ ray array - the National Nuclear Array (NANA). In this study we have sought to exploit the NANA and the excellent timing characteristics of its intrinsic LaBr3(Ce) scintillation detectors for use as a primary standardisation system. For this initial investigation, the absolute standardisation of 60Co has been performed by the γ-γ coincidence technique using NANA and the result compared to the established 4π(LS)-γ Digital Coincidence Counting (DCC) system. The effect of the angular correlation of the stretched E2 transitions emitted from the 4+→2+→0 states of 60Ni on the activity determined by NANA was observed between the pairs of detectors. Corrections for these angular correlations were derived through Monte Carlo simulations. An activity per unit mass by NANA of 330.8 (10) kBqg-1 for the 60Co solution was determined. There was no significant statistical difference between the results of NANA and the 4π(LS)-γ DCC, with a relative difference of 0.04% observed. This study shows that NANA can be used as a primary standard.

Anomalies in the Charge Yields of Fission Fragments from the

Fast-neutron-induced fission of ^{238}U at an energy just above the fission threshold is studied with a novel technique which involves the coupling of a high-efficiency γ-ray spectrometer (MINIBALL) to an inverse-kinematics neutron source (LICORNE) to extract charge yields of fission fragments via γ-γ coincidence spectroscopy. Experimental data and fission models are compared and found to be in reasonable agreement for many nuclei; however, significant discrepancies of up to 600% are observed, particularly for isotopes of Sn and Mo. This indicates that these models significantly overestimate the standard 1 fission mode and suggests that spherical shell effects in the nascent fission fragments are less important for low-energy fast-neutron-induced fission than for thermal neutron-induced fission. This has consequences for understanding and modeling the fission process, for experimental nuclear structure studies of the most neutron-rich nuclei, for future energy applications (e.g., Generation IV reactors which use fast-neutron spectra), and for the reactor antineutrino anomaly.

94 ß-Decay Half-Lives of Neutron-Rich _{55}Cs to _{67}Ho: Experimental Feedback and Evaluation of the r-Process Rare-Earth Peak Formation.

The ß-decay half-lives of 94 neutron-rich nuclei ^{144-151}Cs, ^{146-154}Ba, ^{148-156}La, ^{150-158}Ce, ^{153-160}Pr, ^{156-162}Nd, ^{159-163}Pm, ^{160-166}Sm, ^{161-168}Eu, ^{165-170}Gd, ^{166-172}Tb, ^{169-173}Dy, ^{172-175}Ho, and two isomeric states ^{174m}Er, ^{172m}Dy were measured at the Radioactive Isotope Beam Factory, providing a new experimental basis to test theoretical models. Strikingly large drops of ß-decay half-lives are observed at neutron-number N=97 for _{58}Ce, _{59}Pr, _{60}Nd, and _{62}Sm, and N=105 for _{63}Eu, _{64}Gd, _{65}Tb, and _{66}Dy. Features in the data mirror the interplay between pairing effects and microscopic structure. r-process network calculations performed for a range of mass models and astrophysical conditions show that the 57 half-lives measured for the first time play an important role in shaping the abundance pattern of rare-earth elements in the solar system.

Reference materials produced for a European metrological research project focussing on measurements of NORM.

Reliable measurement of Naturally Occurring Radioactive Materials is of significance in order to comply with environmental regulations and for radiological protection purposes. This paper discusses the standardisation of three reference materials, namely sand, tuff and TiO2 to serve as quality control materials for traceability, method validation and instrument calibration. The sample preparation, material characterization via γ, α and Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and the assignment of values for both the 4n (Thorium) and 4n+2 (Uranium) decay series are described.

Role of the Δ Resonance in the Population of a Four-Nucleon State in the

The ^{54}Fe nucleus was populated from a ^{56}Fe beam impinging on a Be target with an energy of E/A=500 MeV. The internal decay via γ-ray emission of the 10^{+} metastable state was observed. As the structure of this isomeric state has to involve at least four unpaired nucleons, it cannot be populated in a simple two-neutron removal reaction from the ^{56}Fe ground state. The isomeric state was produced in the low-momentum (-energy) tail of the parallel momentum (energy) distribution of ^{54}Fe, suggesting that it was populated via the decay of the Δ^{0} resonance into a proton. This process allows the population of four-nucleon states, such as the observed isomer. Therefore, it is concluded that the observation of this 10^{+} metastable state in ^{54}Fe is a consequence of the quark structure of the nucleons.

Soil radioactivity levels, radiological maps and risk assessment for the state of Kuwait.

An evaluation of the radioactivity levels associated with naturally occurring radioactive materials has been undertaken as part of a systematic study to provide a surface radiological map of the State of Kuwait. Soil samples from across Kuwait were collected, measured and analysed in the current work. These evaluations provided soil activity concentration levels for primordial radionuclides, specifically members of the (238)U and (232)Th decay chains and (40)K which. The (238)U and (232)Th chain radionuclides and (40)K activity concentration values ranged between 5.9 â†” 32.3, 3.5 â†” 27.3, and 74 â†” 698 Bq/kg respectively. The evaluated average specific activity concentrations of (238)U, (232)Th and (40)K across all of the soil samples have mean values of 18, 15 and 385 Bq/kg respectively, all falling below the worldwide mean values of 35, 40 and 400 Bq/kg respectively. The radiological risk factors are associated with a mean of 33.16 ± 2.46 nG/h and 68.5 ± 5.09 Bq/kg for the external dose rate and Radium equivalent respectively. The measured annual dose rates for all samples gives rise to a mean value of 40.8 ± 3.0 µSv/y while the internal and internal hazard indices have been found to be 0.23 ± 0.02 and 0.19 ± 0.01 respectively.

Development of the NPL gamma-ray spectrometer NANA for traceable nuclear decay and structure studies.

We present a brief report on the progress towards the construction of the National Nuclear Array (NANA), a gamma-ray coincidence spectrometer for discrete-line nuclear structure and decay measurements. The proposed spectrometer will combine a gamma-ray energy resolution of approximately 3% at 1MeV with sub-nanosecond timing discrimination between successive gamma rays in mutually coincident decay cascades. We also review a number of recent measurements using coincidence fast-timing gamma-ray spectroscopy for nuclear structure studies, which have helped to inform the design criteria for the NANA spectrometer.

A preliminary evaluation of naturally occurring radioactivity concentration levels across the State of Kuwait.

An evaluation of naturally occurring radioactive materials has been undertaken as part of a systematic study to provide a surface radiological map of the State of Kuwait. Soil samples were collected from twelve locations across Kuwait and analysed using high-resolution gamma-ray spectrometry. The (226)Ra and (235)U specific activity concentrations have been determined and used to estimate the (235)U/(238)U isotopic ratios which are found to be comparable to that expected for naturally occurring uranium material.

Half-life determination of the ground state decay of ¹¹¹Ag.

The radioactive decay half-life of the ß(-)-emitter (111)Ag has been measured using decay transitions identified using a high purity germanium γ-ray spectrometer. The time series of measurements of the net peak areas of the 96.8 keV, 245.4 keV and 342.1 keV γ-ray emissions following the ß(-) decay of (111)Ag were made over approximately 23 days, i.e. ~3 half-life periods. The measured half-life of the ground state decay of (111)Ag was determined as 7.423 (13) days which is consistent with the Evaluated Nuclear Structure Data File (ENSDF) recommended half-life of 7.45 (1) days at k=2. Utilising all available experimental half-life values, a revised recommended half-life of 7.452 (12) days has been determined.

Total Absorption Spectroscopy Study of (92)Rb Decay: A Major Contributor to Reactor Antineutrino Spectrum Shape.

The antineutrino spectra measured in recent experiments at reactors are inconsistent with calculations based on the conversion of integral beta spectra recorded at the ILL reactor. (92)Rb makes the dominant contribution to the reactor antineutrino spectrum in the 5-8 MeV range but its decay properties are in question. We have studied (92)Rb decay with total absorption spectroscopy. Previously unobserved beta feeding was seen in the 4.5-5.5 region and the GS to GS feeding was found to be 87.5(25)%. The impact on the reactor antineutrino spectra calculated with the summation method is shown and discussed.

The half-life of ²²7Th by direct and indirect measurements.

Utilising a chemically purified solution the radioactive half-life of (227)Th has been determined indirectly by observation of the ingrowth of (223)Ra using an ionisation chamber (IC) and for the first time by direct observation of the change in activity with time using a high-purity germanium (HPGe) γ-ray spectrometer. The radioactive decay was observed for ~104 days (~5.6 half-lives) by γ-ray spectrometry and approximately 63 days and 72 days (~3.4 and ~3.9 half-lives) using an ionisation chamber (IC). The resulting half-life values - 18.695 (4) days (IC) and 18.683 (20) days (HPGe) - are consistent and detailed uncertainty budgets are presented for the two measurement techniques. A weighted mean of our results of 18.695 (4) days is inconsistent with the most precise published half-life value of 18.7176 (52) days (Jordan and Blanke, 1967). A critical evaluation of literature data has been performed, indicating a paucity of reliable and independent measurements. Selected independent published values have been used to determine a recommended half-life of 18.697 (7) days. A method has been introduced in the course of this work so that the recommended half-life of (227)Th as determined by ingrowth can be modified if a different (223)Ra half-life has been determined, evaluated and adopted.

Precise measurements of the absolute γ-ray emission probabilities of (223)Ra and decay progeny in equilibrium.

Precise measurements of the absolute γ-ray emission probabilities have been made of radiochemically pure solutions of (223)Ra in equilibrium with its decay progeny, which had been previously standardised by 4π(liquid scintillation)-γ digital coincidence counting techniques. Two high-purity germanium γ-ray spectrometers were used which had been accurately calibrated using a suite of primary and secondary radioactive standards. Comparison of the activity concentration determined by the primary technique against γ-ray spectrometry measurements using the nuclear data evaluations of the Decay Data Evaluation Project exhibited a range of ~18% in the most intense γ-ray emissions (>1% probability) of the (223)Ra decay series. Absolute γ-ray emission probabilities and standard uncertainties have been determined for the decay of (223)Ra, (219)Rn, (215)Po, (211)Pb, (211)Bi and (207)Tl in equilibrium. The standard uncertainties of the measured γ-ray emission probabilities quoted in this work show a significant improvement over previously reported γ-ray emission probabilities. Correlation coefficients for pairs of the measured γ-ray emission probabilities from the decays of the radionuclides (223)Ra, (219)Rn and (211)Pb have been determined and are presented. The α-transition probabilities of the (223)Ra have been deduced from P(γ+ce) balance using the γ-ray emission probabilities determined in this work with some agreement observed with the published experimental values of the α-emission probabilities.