The international reference system for beta-particle emitting radionuclides: Validation through the pilot study CCRI(II)-P1.Co-60.

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.

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.

Half-life determination and comparison of activity standards of 231Pa.

The results of an international comparison of activity measurements of a solution of 231Pa are reported and analysed. Prior to this, no known standardisation of 231Pa by activity measurement had been carried out. The comparison was run in 2017-2018 involving eight laboratories, and returned results with no identifiable inconsistencies between methods or laboratories. The results, including one mass determination, gave a231Pa activity concentration of 41.461(48) kBq g-1 and a231Pa atom concentration of 61.48(23) × 1015 atoms g-1, from which a half-life value of 32 570(130) years was derived.

Preparation and calibration of a 231Pa reference material.

A 231Pa reference material has been characterized for amount of protactinium. This reference material is primarily intended for calibration of 233Pa tracers produced for 235U-231Pa model age measurements associated with nuclear forensics and nuclear safeguards. Primary measurements for characterization were made by isotope dilution mass spectrometry of a purified 231Pa solution using a 233Pa isotopic spike. The spike was calibrated by allowing multiple aliquots of the 233Pa spike solution to decay to 233U and then measuring the ingrown 233U by isotope dilution mass spectrometry using a certified uranium assay and isotopic standard as a reverse-spike. The new 231Pa reference material will simplify calibration of the 233Pa isotope dilution spikes, provide metrological traceability, and potentially reduce the overall measurement uncertainty of model ages.

Defined solid angle alpha counting at NPL.

This paper describes the design of and first measurements with the new defined solid angle (DSA) alpha counter at the National Physical Laboratory, UK, with the aim of enabling high-precision radionuclide standardisations for alpha-emitting radionuclides and half-life measurements. The counter may be employed at three source-detector distances in order to monitor the measured activities with calculated geometrical efficiencies. Initial results are promising but further work is required to reduce the dominant uncertainty associated with the source activity distribution.

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.

Comparison of 9°Y and ¹77Lu measurement capability in UK and European hospitals.

Comparison exercises involving (90)Y and (177)Lu were performed during 2009 and 2012, respectively, to assess the measurement capability of hospitals in the UK and Europe. The results from the measurement of a typical liquid solution of (90)Y show that only 40% of participants could measure the solution to within 5% of the certificated value and that a significant -6% bias was present due to the use of non-standard geometries for the calibration of equipment. The results from the measurement of a standard liquid solution of (177)Lu show that 81% of participants could measure to within 5% of the certificated value and in fact 65% of these results were within 2% of the certificated value, showing administered activities can be far more accurately measured for (177)Lu than for (90)Y and that (177)Lu has a far smaller geometry dependence. These studies were performed to identify specific measurement issues in the user community and to identify areas where future research should be focused. In addition to this the work allows the participants to adjust measurement practice and identify key measurement issues.

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.