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 first official measurement of 11C in the SIRTI.

In the summer of 2017, the Système International de Référence Transfer Instrument (SIRTI) of the Bureau International des Poids et Mesures (BIPM) was hosted by the National Research Council of Canada (NRC) in Ottawa, Canada. This SIRTI visit was unique in many aspects. It was the first visit of the SIRTI to Canada. NRC was the first National Metrological Institute (NMI) to perform comparisons of four isotopes (99mTc, 18F, 64Cu and 11C) during a single two-week period. Finally, this was the first official measurement of 11C in the SIRTI. The NRC had performed a primary standardization of 11C in February of 2017 and calibrated its Secondary Standard Ionizing Radiation Chamber System (SSIRCS) in preparation for the SIRTI comparison. Two primary Liquid Scintillation methods (CIEMAT/NIST and TDCR) were employed and the results agreed. The stock material was received from a local cyclotron in the form of a 11C-labelled sodium acetate (NaC2H3O2). Three ampoules were prepared for the purposes of comparison; one concentrated from the bulk material and two derived from a single dilution. Some inconsistency was evident due to a weighing problem for one of the ampoules containing the diluted solution, whose measurements were excluded from the analysis. The other two ampoules' results were consistent within their respective uncertainties. The SIRTI was very stable and the final BIPM report will detail the stability checks, performance and behaviour of the SIRTI during its measurement campaign in Canada. There is still no Key Comparison Reference Value (KCRV) for 11C as NRC is the first participant. However, during a test of the SIRTI at NPL in 2014, an equivalent SIRTI activity was measured as 9.87(5) kBq which was consistent with MonteCarlo predictions for 11C in the SIRTI of 9.867(15) kBq. The NRC SIRTI equivalent activity for 11C agrees within uncertainty with these results. This offers encouragement to other NMIs to request a 11C comparison given the consistency of experimental results from NRC and test results from the National Physical Laboratory, UK (NPL) and the BIPM. Finally a half-life measurement was determined from the NRC measurement of multiple half-lives of a 11C ampoule and was found to be 20.332(40)min. From the SIRTI measurements at NRC, the half-life was derived as 20.328(13) min. This is smaller but consistent with the DDEP recommended value of 20.361(23)min.

Activity measurements and determination of nuclear decay data of 166Ho in the MRTDosimetry project.

Holmium-166 is a high-energy ß--emitter radionuclide (~ 1.8 MeV) with a short half-life (~26.8h) that offers great potential as an alternative to 90Y for the treatment of liver cancer based on radioembolization. The possibility of quantitative Single Photon Emission Computed Tomography (SPECT) imaging of the main γ-ray emission at 80.6 keV, in addition to strong paramagnetic properties suitable for Magnetic Resonance Imaging (MRI), complement this therapeutic potential. The present paper describes the measurements carried out in three European radionuclide metrology laboratories for primary standardization of 166Ho and new determinations of X- and γ-ray photon-emission intensities in the framework of the European EMPIR project MRTDosimetry. New half-life measurements were also performed.

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.

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.

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.

Results of an international comparison of activity measurements of 68Ge.

An international key comparison, identifier CCRI(II)-K2.Ge-68, has been performed. The National Institute of Standards and Technology (NIST) served as the pilot laboratory, distributing aliquots of a 68Ge/68Ga solution. Results for the activity concentration, CA, of 68Ge at a reference date of 12h00 UTC 14 November 2014 were submitted by 17 laboratories, encompassing many variants of coincidence methods and liquid-scintillation counting methods. The first use of 4π(Cherenkov)ß-γ coincidence and anticoincidence methods in an international comparison is reported. One participant reported results by secondary methods only. Two results, both utilizing pure liquid-scintillation methods, were identified as outliers. Evaluation using the Power-Moderated Mean method results in a proposed Comparison Reference Value (CRV) of 621.7(11)kBqg-1, based on 14 results. The degrees of equivalence and their associated uncertainties are evaluated for each participant. Several participants submitted 3.6mL ampoules to the BIPM to link the comparison to the International Reference System (SIR) which may lead to the evaluation of a Key Comparison Reference Value and associated degrees of equivalence.

Activity measurements of the radionuclides 18F and 64Cu for the NIST, USA in the ongoing comparisons BIPM.RI(II)-K4.F-18 and BIPM.RI(II)-K4.Cu-64.

In 2016, comparisons of activity measurements of 18F and 64Cu using the Transfer Instrument of the International Reference System (SIRTI) took place at the National Institute of Standards and Technology (NIST, USA). This is the first SIRTI comparison for 64Cu. Ampoules containing about 27 kBq of 18F and 100 kBq of 64Cu solutions were measured in the SIRTI for about 5 and 1.5 half-lives, respectively. The NIST standardized the activity in the ampoules by ionization chamber measurements traceable to 4π(LS)ß-γ anticoincidence measurements. The comparisons, identifiers BIPM.RI(II)-K4.F-18 and BIPM.RI(II)-K4.Cu-64, are linked to the corresponding BIPM.RI(II)-K1.F-18 and BIPM.RI(II)-K1.Cu-64 comparisons and degrees of equivalence with the respective key comparison reference values have been evaluated. The NIST replaces its earlier degree of equivalence for 18F obtained in the frame of the CCRI(II)-K3.F-18 comparison in 2001.

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.

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.

Modeling the transmission of beta rays through thin foils in planar geometry.

This paper is concerned with the modeling of the transmission of beta rays through thin foils in planar geometry based on the plane source concept, using Monte Carlo simulation of electron transport and least squares fitting. Applications of modeling results for calculating the efficiency of large-area beta sources, transmission coefficient of beta rays through thin foils and the beta detection efficiency of large-area detectors used in surface contamination measurements are also presented.

A novel method for the activity measurement of large-area beta reference sources.

A novel method has been developed for the activity measurement of large-area beta reference sources. It makes use of two emission rate measurements and is based on the weak dependence between the source activity and the activity distribution for a given value of transmission coefficient. The method was checked experimentally by measuring the activity of two ((60)Co and (137)Cs) large-area reference sources constructed from anodized aluminum foils. Measurement results were compared with the activity values measured by gamma spectrometry. For each source, they agree within one standard uncertainty and also agree within the same limits with the certified values of the source activity.

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.

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.

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.

Results of an international comparison for the activity measurement of 177Lu.

An international Key Comparison of (177)Lu has recently been carried out. Twelve laboratories performed assays for radioactivity content on aliquots of a common master solution of (177)Lu, leading to eleven results submitted for entry into the Key Comparison Database of the Mutual Recognition Arrangement. A proposed Comparison Reference Value (CRV) was calculated to be 3.288(4)MBq/g using all eleven results. Degrees of equivalence and their uncertainties were calculated for each laboratory based on the CRV. Most of the values reported by the participating laboratories were within 0.6% of the CRV.

Standardization, decay data measurements and evaluation of 64Cu.

The purposes of this study were to create national activity standards of (64)Cu, to make possible the definition of an international key comparison reference value and to determine the decay data in order to improve the decay scheme. Four laboratories measured the activity of a (64)Cu solution; these results were compared through the International Reference System. Moreover, the laboratories carried out new measurements of the photon emission intensities and of the half-life. A new decay scheme was derived from these new values and the previously published ones.

Cerebral thromboembolic events in pediatric patients with inflammatory bowel disease.

BACKGROUND: There is a recognized association between pediatric inflammatory bowel disease (IBD) and cerebral thromboembolic events (CTEs). Historical reporting had described the association as strongest between ulcerative colitis (UC), rather than Crohn's disease (CD). We describe the incidence and outcome of CTE in pediatric IBD patients from a single center over 5 years and the relative proportion of stroke reported in the literature in patients with UC and CD before and after January 2000. METHODS: Demographic data were extracted on all newly diagnosed cases of IBD in our center from January 2003 to January 2008 to ascertain patient characteristics, disease type, risk factors for CTE, modality of neuroimaging, and outcome. A literature search was performed to identify all articles describing stroke in pediatric IBD. All identified studies were stratified into those published before and after January 1 2000. RESULTS: In all, 154 new patients diagnosed with IBD (male 56%) (UC 30%, CD 64%, IBD unclassified [IBDU] 6%) were reviewed. Four cases of CTE occurred in our population over 5 years (2.6%). All patients had a risk factor for CTE. Fifteen case series were identified with 32 patients. There was a significant increase in the proportion strokes affecting patients with CD reported after January 2000 (P = 0.02). CONCLUSIONS: CTE affects a proportion of pediatric IBD patients. Although resolution of physical impairment is the norm, significant morbidity exists. Our study suggests a secular trend toward CTE in CD. Primary prevention with the identification and amelioration of identifiable risk factors should be the clinical objective in future studies.