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).

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.

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.

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.

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.

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.

An approach based on the SIR measurement model for determining the ionization chamber efficiency curves, and a study of 65Zn and 201Tl photon emission intensities.

The measurement model used to determine ionization chamber efficiency curves accounts from the outset for impurity corrections and beta spectrum shapes. The curves are represented by exponentials of polynomials whose coefficients are adjusted using non-linear least-squares minimization. The curves are validated by comparing with SIR key comparison reference values (KCRVs) and other published curves. The associated covariance matrix is also evaluated. Deviations from model predictions for 65Zn and 201Tl using recommended nuclear data are studied.

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.

Secondary standardisation of 95mTc.

The radionuclide 95mTc, which has a half-life of 61(2)days and emits a number of gamma-rays, may be used in radiochemical analysis as a yield tracer for the long-lived fission product 99Tc. In this work, we present (i) the production of 95mTc via an (alpha, 2n) reaction with stable 93Nb (a method which does not result in the production of any 97mTc, 98Tc or 99Tc), (ii) the chemical separation of 95mTc from niobium via coprecipitation, liquid-liquid extraction and liquid chromatography, and (iii) the secondary standardisation of 95mTc with high-resolution gamma-ray spectrometry and an ionisation chamber system.

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.

Integrating stress-response and cell-cycle checkpoint pathways.

The DNA integrity checkpoint and stress kinase (SAPK/JNK and p38) pathways function to modulate cell-cycle, apoptotic and transcriptional responses to stress. Although initially considered to function independently, recent advances indicate a number of links between the stress-response and checkpoint pathways. Here, we consider the relationship between the stress-response and checkpoint pathways and how they interact to modulate cell-cycle control.