S.M. Collins

Direct measurement of the half-life of 223Ra

Radioactive decay half-life measurements of (223)Ra, a member of the (235)U naturally occurring radioactive decay series, have been performed of a radiochemically pure solution with an ionisation chamber. The radioactive decay of (223)Ra was followed for 50 days, approximately 4.4 half-lives. The deduced half-life of (223)Ra was found to be 11.4358 (28) days, supporting the other published direct measurements. A detailed uncertainty budget is presented. A new evaluation of the published half-life values was performed, indicating significant variation across the existing published values, suggesting that further measurements of the half-life of (223)Ra are required. A new evaluated half-life has been calculated using a power moderated weighted mean of selected experimental values, with a new value of the recommended half-life for (223)Ra of 11.4354 (17) days.

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.

Standardisation of 223Ra by liquid scintillation counting techniques and comparison with secondary measurements

An aqueous solution of 223Ra chloride in equilibrium with its decay progeny was standardised by liquid scintillation counting techniques. Since secular equilibrium with the decay progeny of 223Ra had been established by the time of measurement, the apparent detection efficiency of 223Ra was approximately 6 and was determined by both the CIEMAT/NIST efficiency tracing technique and the 4π(LS)-γ digital coincidence counting techniques. The results obtained were compared with γ-spectrometry and ionisation chamber measurements. Whilst the γ-spectrometry measurements were in agreement (albeit exhibiting a large spread (18%) in the individual activity estimations using the main γ-emissions), a significant discrepancy of the order of 9% was identified between the liquid scintillation counting results and those obtained using published calibration factors for a variety of radionuclide calibrators.

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.

Unbiased equations for 95Zr–95Nb chronometry

Formulae are presented for (95)Zr-(95)Nb chronometry of a nuclear event. In particular, they allow for a bias-free calculation of the moment of a nuclear explosion, based solely on a measurement of the produced activity ratio of (95)Zr and (95)Nb in a finite time interval. Also uncertainty propagation factors are presented, which relate the relative uncertainty on the nuclear decay data and activity ratio measurements with the relative uncertainty on the elapsed time. This allows for the calculation of an uncertainty budget, without the need for Monte Carlo simulations. The equations are applied to a set of measurement data and consistency is demonstrated.

Migration to new ampoule types for the NPL secondary standard ionisation chambers.

As the pre-calibrated sample containers used for activity assay in the two NPL secondary standards ionisation chambers are being phased out, suitable replacements have been identified. Characterisation checks have been carried out on the new ISO ampoules and a long-term recalibration schedule has been devised. Around 40 calibration factors have been determined so far and comparison of ion chamber responses for the two ampoule types showed variations of up to 7% for low energy photon emitting radionuclides.

Determination of the gamma emission intensities of 111Ag

A radioactive solution of (111)Ag, standardised by the absolute measurement methods 4π(PC)-γ and 4π(LS)-γ coincidence counting at the National Physical Laboratory (NPL), was measured by two independently calibrated HPGe γ spectrometers in order to estimate the γ emission intensities and to determine the absolute intensity, with the aim of improving the currently published values. An absolute intensity value of 6.68 (7)% was obtained for the 342.1 keV γ emission, which is in agreement with previously reported values, but greatly reduces the uncertainty. Additionally, this work proposes a new emission intensity for the 450.0 keV γ emission that has not been previously reported, with an absolute intensity of 0.000482 (12)%. An investigation of the published γ emission intensities shows significant discrepancies that require resolution.

A comparison of emerging gamma detector technologies for airborne radiation monitoring

This paper presents a comparison of new and emerging gamma detector technologies that have the potential to improve in-situ dose and radioactivity-in-air measurements for national monitoring networks. Five detectors were chosen for investigation; LaBr3(Ce), CeBr3, SiPM-CsI(Tl), Cd(Zn)Te and electromechanically-cooled HPGe. These detectors represent the full range of the price-performance matrix. Comparisons have been made of energy resolution, detection efficiency and minimum detectable activity by exposing each detector to a mixed radionuclide source drop-deposited across a filter. Other factors, such as internal radioactivity, linearity, size and cost have also been considered.

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.

Development of NANA: A Fast-Scintillator, Coincidence Gamma-ray Array for Radioactive Source Characterisation and Absolute Activity Measurements at the UK National Physical Laboratory

A multi-detector modular coincidence gamma-ray spectrometer is being designed and constructed for use at the UKs National Physical Laboratory (NPL) for use in direct measurement and metrological standardisation of nuclear decay activities. In its first generation, the NPL National Nuclear Array (NANA) will consist of twelve individual halide scintillation detectors placed in a high-efficiency geometry around a well-defined central point source position. This brief conference paper provides details of the measured detector module and coincidence energy and timing responses for the LaBr3(Ce) detectors which will be used in the NANA array. Preliminary GEANT4 simulations of the arrays full energy peak efficiency and expected gamma-ray coincidence response are also presented.