Standardisation of 231Pa by defined solid angle and liquid scintillation methods at NPL.

231Pa is the longest-lived decay product in the 235U decay chain and precise standards of this radionuclide are required to enable accurate, traceable measurements in nuclear dating applications such as geochronometry and nuclear forensics. Three independent techniques were used at NPL to determine the activity per unit mass of a freshly separated 231Pa solution as part of an international CCRI(II) comparison: CCRI(II)-K2.Pa-231.The first method was defined solid angle α counting and is the first result reported in a BIPM comparison with this instrument. The second method was 4πα liquid scintillation (LS) counting combined with the CIEMAT/NIST method using commercially available LS counters. The third technique used was 4π(LS)α-γ coincidence counting on an NPL-built system comprising an LS counter with dual photomultiplier tubes (PMTs) coupled to a 70% relative efficiency HPGe γ-spectrometer. Excellent agreement between the three methods was obtained.

The potential radio-immunotherapeutic α-emitter 227Th - part II: Absolute γ-ray emission intensities from the excited levels of 223Ra.

At the time of publication, radiopharmaceuticals labelled with thorium-227 are in clinical trials in Europe for the treatment of various types of cancer. In part I of this two-part series the primary standardisation of an aqueous solution of 227Th was reported. In part II, the activity derived from the recommended absolute γ-ray emission intensities have been compared to that from the primary standardisation techniques. This comparison showed a negative bias of 4% in the determined activity per unit mass with an 11% spread in the activities determined for the eight most intense γ-ray emissions (Iγ > 1%) from the 227Th α decay. Using the standardised 227Th, measurements of the characteristic γ-ray emissions from the 223Ra excited states were made using a calibrated HPGe γ-ray spectrometer. This has enabled the absolute intensities of 70 γ ray emissions from the 227Th α-decay to be experimentally determined. A significant improvement over the precision of the recommended normalisation scaling factor has been made, with a value of 12.470 (35) % determined. Typically, the precision of the intensities has been improved by an order of magnitude or greater than current recommended values. The correlation matrices for pairs of the most intense γ-ray emission intensities are presented.

The potential radio-immunotherapeutic α-emitter 227Th - part I: Standardisation via primary liquid scintillation techniques and decay progeny ingrowth measurements.

Thorium-227 is a potential therapeutic radionuclide for applications in targeted α-radioimmunotherapy for the treatment of various types of cancer. To provide nuclear medicine departments involved in Phase I clinical trials traceability to the SI unit of radioactivity (Bq), a standardisation of a radiochemically pure 227Th aqueous solution has been performed at the National Physical Laboratory. This was achieved via two primary liquid scintillation (LS) techniques -4π(LS)-γ digital coincidence counting (DCC) and 4π LS counting. These absolute techniques were supported by the indirect determination of the 227Th activity via the measurement of the ingrowth and decay rate of the decay progeny by both ionisations chambers and high purity germanium (HPGe) gamma-ray spectrometry. The results of the primary techniques were found to be consistent, both with each other (zeta score = 1.1) and to the decay progeny ingrowth measurements. An activity per unit mass of 20.726 (51) kBq g-1 was determined for the solution. A procedure has been developed that provided an effective separation of the 227Th from its decay progeny, which was shown by the effective time zero of the 227Th-223Ra nuclear chronometer measured by HPGe gamma-ray spectrometry.

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.

Is decay constant?

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, ß-, ß+ 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.

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.

Comparison of (18)F activity measurements at the VNIIM, NPL and the ENEA-INMRI using the SIRTI of the BIPM.

In 2014, the first three comparisons of activity measurements of (18)F were carried out at the VNIIM, NPL and the ENEA-INMRI using the BIPM's Transfer Instrument of the International Reference System. The transfer instrument and the NMIs primary measurement methods are briefly described. The degrees of equivalence with the key comparison reference value defined in the frame of the corresponding SIR comparison have been evaluated. World-wide consistency of activity measurements of (18)F is demonstrated.

Evidence against solar influence on nuclear decay constants.

The hypothesis that proximity to the Sun causes variation of decay constants at permille level has been tested and disproved. Repeated activity measurements of mono-radionuclide sources were performed over periods from 200 days up to four decades at 14 laboratories across the globe. Residuals from the exponential nuclear decay curves were inspected for annual oscillations. Systematic deviations from a purely exponential decay curve differ from one data set to another and are attributable to instabilities in the instrumentation and measurement conditions. The most stable activity measurements of alpha, beta-minus, electron capture, and beta-plus decaying sources set an upper limit of 0.0006% to 0.008% to the amplitude of annual oscillations in the decay rate. Oscillations in phase with Earth's orbital distance to the Sun could not be observed within a 10-6 to 10-5 range of precision. There are also no apparent modulations over periods of weeks or months. Consequently, there is no indication of a natural impediment against sub-permille accuracy in half-life determinations, renormalisation of activity to a distant reference date, application of nuclear dating for archaeology, geo- and cosmochronology, nor in establishing the SI unit becquerel and seeking international equivalence of activity standards.

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.

Direct measurement of the half-life of (223)Ra.

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.

Primary standardisation of 204Tl using the efficiency tracing method.

The electron-capture and beta(-) -emitting radionuclide 204Tl has been known from previous experience to show discrepancies between different methods of standardisation. Source preparation is also difficult due to the complex chemistry of thallium. The Bureau International des Poids et Mesures (BIPM) intercomparison held in 1997, showed discrepancies of up to 10% between measurements of solid sources and liquid scintillation methods. These problems have been the subject of a BIPM CCRI(II) working group since 1999. This paper presents the results from a primary standardisation of a 204Tl solution using 4pibeta-gamma coincidence counting and liquid scintillation counting. The tracer technique was used for the 4pibeta-gamma coincidence counting, where 204Tl was traced with 134Cs and 60Co. The extrapolation to 100% beta-efficiency was performed by three different approaches: foiling, adding carrier and measuring sources of different initial masses. The results showed that tracing with 60Co and using external foiling gave the same result as obtained by liquid scintillation counting. A comparison of the results achieved by the different methods of measurement, tracers and methods for extrapolation is presented and discussed in this paper.

Standardisation of 11C.

The increasing use of positron emission tomography for medical imaging and the availability of short-lived positron emitters has raised concerns about the accuracy of calibration of secondary standard measurement systems and the viability of using a single long-lived positron emitter as a reference calibration source for all positron emitters. Potential problems arise because the 511 keV quanta arising from positron annihilation are not generally produced at the same point as the original disintegration. In addition, the secondary standard may also be responsive to the associated bremsstrahlung radiation. The magnitude of both effects depends on the positron end-point energy. In order to resolve these problems, it is necessary to produce absolute standards of these positron-emitting radionuclides and the work presented here details the results of such work with 11C.