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IRA recently launched a project to digitize all the data acquisition systems it uses for primary radionuclide standardizations. It is well-known that the digital approach presents numerous advantages over the traditional analog electronics such as information losslessness, scalability, online and/or offline data processing, and it is also a solution to the growing difficulties to repair or renew ageing modules. As a first step in this wider program, our institute set-up a 4πβ-4πγ digital coincidence counting system, with FPGA (Field Programmable Gate Array)-based commercial boards from National Instruments (NI), to perform data acquisition and offline data analysis. Choosing all components and software from the same supplier provides a full compact and consistent electronic system. To demonstrate and validate the capacity of this system to standardize the activity of radioisotopes, we compare its predictions for the activity concentration of 133Ba, 166mHo and 18F solutions with the results from a coincidence counting system with analog electronics, as well as with the results from other primary methods and a secondary measurement performed with an IG11 ionization chamber (CIR, chambre d'ionization de reference) with an equivalent activity traceable to the Systeme International de Reference.

The gamma and X-ray emission intensities of 169Er were determined using radionuclidically pure 169Er. The activity of the 169Er source was standardized by the triple-to-double-coincidence ratio technique. Three independent measurements were performed to measure the emission intensities using calibrated high-purity germanium spectrometers. The efficiencies were computed with the Monte Carlo method and validated using several experimental measurements. Final results present a large uncertainty reduction compared to previous evaluations. The emission intensities per decay of 169Er are reported as 1.401(40).10−5 for the 109.8 keV line and 1.513(19).10−6 for the 118.2 keV line. The values obtained for the X-ray lines show large discrepancies with the reference values.

We report here on the primary activity standardisation of a223Ra dichloride solution in equilibrium with its decay daughters. Both the triple-to-double-coincidence-ratio (TDCR) method with an in-house TDCR detector and the CIEMAT-NIST efficiency tracing (CNET) technique with a commercial counter were used. The liquid scintillation efficiencies for both methods are about 6 while the activities they predict with about 0.4% relative standard uncertainty agree within 0.15%. For backup, the solution was also standardised with 4πγ NaI(Tl) integral counting with a well-type NaI(Tl) detector, and efficiencies computed by Monte Carlo simulations using the GEANT code. This simple technique, unused previously for this nuclide, yielded an activity concentration compatible with, but 1% lower than, the one determined by liquid scintillation counting.

This work looks into the tracks of electrons in nanoemulsive scintillating media using the Monte Carlo Geant4-DNA code which simulates event-by-event interactions of electrons in liquid water down to the eV, without resorting to the condensed history method. It demonstrates that the average number of micelles in which electrons deposit energy is quite large, increasing with their emission energy, decreasing with micelle size, and rising with micelle concentration. The probability of an electron ending its track in a micelle is found to be rather large and micelle size-dependent below 1 keV, and approximating the aqueous fraction at higher energies. Analyses of the Monte Carlo estimated energy depositions in the aqueous phase and in the scintillant tell of a micelle quenching effect, with the micelle size shaping the quenching at low energy and the micelle concentration governing it at higher energies. The micelle effect on the 3 H and 63 Ni beta spectra is discussed for a range of micelle sizes and concentrations. This paper also computes the ionisation quenching function using Birk's law whilst considering the full energy losses in the micelles bisecting the electron pathway, and not just that incurred in the primary micelle enclosing the decaying nuclide. The ionisation quenching function is then used to calculate the detection efficiencies for 3 H, 63 Ni, 54 Mn and 55 Fe. The effect of the micelle size is found to be small for beta emitters but significant for the electron capture nuclides. TDCR measurements of 63 Ni samples covering 8 aqueous fractions are analysed with and without explicit treatment of the micelle effect. Activities in the two representations agree within 0.02%. The ratios of the corresponding figures of merit are found to coincide with the scintillant fractions.

The half-life of 137Cs was measured with an ionization chamber by following the decay of 5 sources over a 30 years period between 1983 and 2013. The ratio between the ionization chamber current for the cesium sources and 226Ra source was used for the half-life calculation. The value found for the 137Cs half-life is 10,955.2±10.7 days, where the uncertainty evaluation combines type A and B for one standard deviation.

The stability of 3H and 63Ni samples, made with Ultima Gold and Ultima Gold AB using eight aqueous fractions ranging between 0.1% and 10%, was monitored over a period of 32 weeks. Counting rate losses were measured in all cases, but were found to be particularly severe for samples with low aqueous fractions. Hydrodynamic diameter measurements of the reverse micelles of 3H and 63Ni in Ultima Gold and Ultima Gold AB samples were performed with dynamic light scattering. For Ultima Gold, the micelle diameters were measured to be about 2nm and slightly dependent of the aqueous fraction, while for Ultima Gold AB they were found to vary strongly with the aqueous fraction and range between 1 and 4nm. The hypothesis that the counting rate instabilities derive from changes in the sizes of micelles was tested by measuring them four times over the monitoring period. The measurement results do not support this claim.

161Tb, which emits low-energy β−- and γ-particles in addition to conversion and Auger electrons, has aroused increased interest for medical imaging and therapy. To support the use of this radionuclide, a161Tb solution was standardised using the β-γ coincidence technique, as well as the TDCR method. The solution had 4.5·10−3% of 160Tb impurities. Primary coincidence measurements, with plastic or liquid scintillators for beta detection, were carried out using both analogue and digital electronics. TDCR measurements using defocusing, grey filtering and quenching for varying the efficiency were also made. Monte Carlo calculations were used to compute the detection efficiency. The coincidence measurements with analogue electronics and the TDCR show a good consistency, and are compatible with the digital coincidence results within uncertainties. An ampoule of this solution was submitted to the BIPM as a contribution to the international reference system.

The radiolanthanide 161Tb is being studied as an alternative to 177Lu for targeted radionuclide tumor therapy. Both β--particle emitters show similar chemical behavior and decay characteristics, but 161Tb delivers additional conversion and Auger electron emissions that may enhance the therapeutic efficacy. In this study, the half-life of 161Tb was determined by a combination of three independent measurement systems: reference ionization chamber (CIR, chambre d'ionization de reference), portable ionization chamber (TCIR) and a CeBr3 γ-emission detector with digital electronics. The half-life determined for 161Tb is 6.953(2) days, showing a significant improvement in the uncertainty, which is one order of magnitude lower, with a deviation of 0.91% from the last nuclear data reference value. The previous large uncertainty of the half-life had a direct impact on activity measurements. Now it is no more an obstacle to a primary standardization.

The radioactive concentrations of (166m)Ho, (134)Cs and (133)Ba solutions have been standardised using a 4πβ-4πγ coincidence counting system we have recently set up. The detection in the beta channel is performed using various geometries of a UPS-89 plastic scintillator optically coupled to a selected low-noise 1in. diameter photomultiplier tube. The light-tight thin capsule that encloses this beta detector is housed within the well of a 5in.×5in. NaI(Tl) monocrystal detector. The beta detection efficiency can be varied either by optical filtering or electronic discrimination when the electrons loose all their energy in the plastic scintillator. This 4πβ-4πγ coincidence system improves on our 4πβ(PC)-γ system in that its sample preparation is less labour intensive, it yields larger beta- and gamma-counting efficiencies thus enabling the standardisation of low activity sources with good statistics in reasonable time, and it makes standardising short-lived radionuclides easier. The resulting radioactive concentrations of (166m)Ho, (134)Cs and (133)Ba are found to agree with those measured with other primary measurement methods thus validating our 4πβ-4πγ coincidence counting system.

An international exercise, registered as EUROMET project no. 907, was launched to measure both the activity of a solution of (124)Sb and the photon emission intensities of its decay. The same solution was sent by LNE-LNHB to eight participating laboratories. In order to identify possible biases, the participants were asked to use all possible activity measurement methods available in their laboratory and then to determine their reference value for comparison. Thus, measurement results from 4pibeta-gamma coincidence/anti-coincidence counting, CIEMAT/NIST liquid-scintillation counting, 4pigamma counting with well-type ionization chambers and well-type crystal detectors were given. The results are compared and show a maximum discrepancy of about 1.6%: possible explanations are proposed.

The activity of radiopharmaceuticals in nuclear medicine is measured before patient injection with radionuclide calibrators. In Switzerland, the general requirements for quality controls are defined in a federal ordinance and a directive of the Federal Office of Metrology (METAS) which require each instrument to be verified. A set of three gamma sources (Co-57, Cs-137 and Co-60) is used to verify the response of radionuclide calibrators in the gamma energy range of their use. A beta source, a mixture of 90 Sr and 90 Y in secular equilibrium, is used as well. Manufacturers are responsible for the calibration factors. The main goal of the study was to monitor the validity of the calibration factors by using two sources: a 90 Sr/ 90 Y source and a 18 F source. The three types of commercial radionuclide calibrators tested do not have a calibration factor for the mixture but only for 90 Y. Activity measurements of a 90 Sr/ 90 Y source with the 90 Y calibration factor are performed in order to correct for the extra-contribution of 90 Sr. The value of the correction factor was found to be 1.113 whereas Monte Carlo simulations of the radionuclide calibrators estimate the correction factor to be 1.117. Measurements with 18 F sources in a specific geometry are also performed. Since this radionuclide is widely used in Swiss hospitals equipped with PET and PET-CT, the metrology of the 18 F is very important. The 18 F response normalized to the 137 Cs response shows that the difference with a reference value does not exceed 3% for the three types of radionuclide calibrators.

As part of a project to use the long-lived (T(1/2)=1200a) (166m)Ho as reference source in its reference ionisation chamber, IRA standardised a commercially acquired solution of this nuclide using the 4pibeta-gamma coincidence and 4pigamma (NaI) methods. The (166m)Ho solution supplied by Isotope Product Laboratories was measured to have about 5% Europium impurities (3% (154)Eu, 0.94% (152)Eu and 0.9% (155)Eu). Holmium had therefore to be separated from europium, and this was carried out by means of ion-exchange chromatography. The holmium fractions were collected without europium contamination: 162h long HPGe gamma measurements indicated no europium impurity (detection limits of 0.01% for (152)Eu and (154)Eu, and 0.03% for (155)Eu). The primary measurement of the purified (166m)Ho solution with the 4pi (PC) beta-gamma coincidence technique was carried out at three gamma energy settings: a window around the 184.4keV peak and gamma thresholds at 121.8 and 637.3keV. The results show very good self-consistency, and the activity concentration of the solution was evaluated to be 45.640+/-0.098kBq/g (0.21% with k=1). The activity concentration of this solution was also measured by integral counting with a well-type 5''x5'' NaI(Tl) detector and efficiencies computed by Monte Carlo simulations using the GEANT code. These measurements were mutually consistent, while the resulting weighted average of the 4pi NaI(Tl) method was found to agree within 0.15% with the result of the 4pibeta-gamma coincidence technique. An ampoule of this solution and the measured value of the concentration were submitted to the BIPM as a contribution to the Système International de Référence.