The operation of an ionization chamber with depleted gas for radioactivity measurement: Calibration procedure and utilising normalized manufacturer's radionuclide factors.

At the National Metrology Institute of South Africa (NMISA) absolute activity measurements of γ-emitting radionuclides are maintained for longevity on a secondary standard ionization chamber. Because the ionization chamber has lower gas pressure than that normally produced by the manufacturer, this paper focuses attention on explaining a normalization scheme devised to allow NMISA to make use of the manufacturer's supplied radionuclide calibration factors when necessary. The applicability of the procedure is justified through analysis of some results from a comprehensive simulation of the chamber undertaken in an independent study. Comparisons of the derived normalized calibration factors against those obtained through measurement at NMISA are made for a variety of radionuclides.

Activity determination of 18F using liquid scintillation beta-efficiency extrapolation and non-extrapolation methods.

The absolute activity of 18F was determined using 4πß-γ liquid scintillation coincidence counting using beta-efficiency extrapolation. An ionization chamber factor was determined for use during a SIRTI comparison, for which results are presented. A non-extrapolation method based on a detection efficiency analysis was also employed using an adaptation of the double-phototube coincidence efficiency for a threshold above the second monopeak. Results and uncertainty budgets for the two methods are presented and discussed.

Absolute standardizations of 99mTc and 57Co by 4π electron-gamma liquid scintillation coincidence counting for SIRTI and SIR comparisons.

The radionuclides 99mTc and 57Co were standardized via absolute liquid scintillation counting techniques. We provide the first technical report on the absolute standardization of 99mTc using 4π(LS)e-γ coincidence counting. The low detection efficiency of low-energy conversion electrons translates into a large efficiency extrapolation range. A simulation indicated that the γ-ray interacting with the liquid scintillator introduces curvature to the count rate vs. efficiency relationship, the approximation of the functional form used for extrapolation providing the main measurement uncertainty for 99mTc. A detection efficiency analysis for both radionuclides is presented. Results from the standardizations, and SIRTI and SIR comparison exercises are reported.

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.

Activity determination of (59)Fe by 4π beta-gamma counting using liquid scintillation in the beta channel.

This paper reports on absolute activity measurements of iron-59 made at the National Metrology Institute of South Africa (NMISA) via 4π(LS)ß-γ coincidence counting. The exercise formed part of an Asia Pacific Metrology Program (APMP) regional key comparison. Source data were analysed by the extrapolation technique for a number of gamma-ray window settings. In addition, a feasibility study was undertaken on a second technique; a non-extrapolation method based on a detection efficiency analysis. The reported activity concentration of the (59)Fe solution was determined with a relative uncertainty of 0.28% (k=1), the uncertainty being due mainly to the rate vs. efficiency fitting process. The result from the non-extrapolation method was lower than that given by extrapolation by 0.33%, within two standard deviations. Possible reasons for the small discrepancy are discussed.

Standardization of Tc-99 by three liquid scintillation counting methods.

The NMISA participated in the international key comparison of the pure beta-emitter Technetium-99, CCRI(II)-K2.Tc-99. The comparison solution was standardized using three methods, namely the TDCR efficiency calculation method, the CIEMAT/NIST efficiency tracing method and the 4π(LS)ß-γ coincidence tracing method with Co-60 as tracer. Excellent agreement between results obtained with the three methods confirmed the applicability of the beta spectral shape given by the latest (2011) DDEP evaluation of Tc-99 decay data, rather than the earlier (2004) evaluation.

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.

Accurate activity measurement of Lu-177 by the liquid scintillation 4πß-γ coincidence counting technique.

This paper reports on absolute measurements made at the NMISA by the 4π[LS]ß-γ coincidence extrapolation technique, which formed part of a key comparison of activity measurements of the radionuclide lutetium-177, a beta-gamma emitter. A detection efficiency analysis based on the decay scheme indicated that the coincidence extrapolation method is feasible for extracting the source disintegration rate of (177)Lu. A simulation was undertaken utilizing the efficiency equations to give an indication of the expected variation of the source count rate with efficiency for different gamma-ray windows. Both the simulation and experiment indicated that the window giving the highest counting efficiency was centered about the 208.4 keV photopeak, with the data showing linear variation in the upper efficiency range. The extracted activity concentration of the (177)Lu solution proved to be highly accurate, being higher than the proposed comparison reference value by 0.15%, well within one standard uncertainty (σ=0.26%) as specified by the NMISA.

Absolute standardization of 241Pu by the TDCR technique and effect of the beta spectral shape.

The NMISA participated in the 2010 international key comparison of (241)Pu, standardizing the inter-comparison solution by the TDCR efficiency calculation technique. Special attention was paid to ensure accurate efficiency calculation for this low-energy, pure beta-emitter: in particular the effect of low-energy stopping powers on the calculation of ionization quenching was assessed and an optimal value for the quench parameter, kB, was determined. In addition, phototube efficiency mismatch was accounted for by a software minimization technique. The effect of the beta spectral shape on the activity extracted from data analysis was assessed and found to be significant. Based on the results of this work we propose a new value for the average beta-particle energy.

Fe-55 activity measurements at the NMISA revisited.

Twenty years ago South Africa's Radioactivity Standards Laboratory (now operated by the NMISA) was the first to measure the activity of (55)Fe by combining the triple-to-double coincidence ratio (TDCR) liquid scintillation method with theoretical efficiency formulae. The extracted activity was however found to be consistently low by about 6%. Due to improvements in both the counting system and analysis technique, it was decided to re-examine the method as applied at the NMISA. The latest results are presented and discussed, particularly with regard to a quantitative study into which vial type is better suited to obtaining accurate (55)Fe activity measurements.

Absolute activity of (133)Ba by liquid scintillation coincidence counting using the 4pi(e,X)-gamma extrapolation technique.

The Technical Committee for Ionizing Radiation (TCRI) of the Asia Pacific Metrology Programme (APMP) recently organized a regional key comparison of activity measurements of the radionuclide (133)Ba. This paper reports on absolute measurements made at the National Metrology Institute of South Africa (NMISA) by the coincidence extrapolation technique, with liquid scintillation counting (LSC) comprising the 4pi channel. A detection efficiency analysis was undertaken to predict the maximum efficiency likely to be achieved and to confirm that the method does indeed provide the source disintegration rate for (133)Ba. Various experimental and data analysis difficulties to be aware of are discussed in the paper.

Further investigations of a simple counting technique for measuring mixtures of two pure beta-emitting radionuclides.

A simple liquid scintillation counting technique to measure the activity composition of a mixture containing two known pure beta-emitting radionuclides was recently developed at the NMISA. The method has been applied to various two-component mixtures of (32)P, (33)P and (35)S, primarily to gauge the effect of spectral energy differences on the method's ability to extract the individual activities. Excellent results were obtained for mixtures of (33)P and (35)S, radionuclides with similar, low beta energies. Mixtures containing the high-energy beta-emitter (32)P were more difficult to resolve, although quenching of the counting sources with CHCl(3) improved mixture resolution.

Comparison of calculated spectra for the interaction of photons in a liquid scintillator. Example of 54Mn 835 keV emission.

The CIEMAT/NIST and TDCR methods in liquid scintillation counting, initially developed for the activity standardization of pure-beta radionuclides, have been extended to the standardization of electron capture and beta-gamma radionuclides. Both methods require the calculation of the energy spectrum absorbed by the liquid scintillator. For radionuclides emitting X-rays or gamma-rays, when the energy is greater than a few tens of keV the Compton interaction is important and the absorption is not total. In this case, the spectrum absorbed by the scintillator must be calculated using analytical or stochastic models. An illustration of this problem is the standardization of 54Mn, which is a radionuclide decaying by electron capture. The gamma transition, very weakly converted, leads to the emission of an 835 keV photon. The calculation of the detection efficiency of this radionuclide requires the calculation of the energy spectrum transferred to the scintillator after the absorption of the gamma ray and the associated probability of absorption. The validity of the method is thus dependent on the correct calculation of the energy transferred to the scintillator. In order to compare the calculation results obtained using various calculation tools, and to provide the metrology community with some information on the choice of these tools, the LS working group of the ICRM organised a comparison of the calculated absorbed spectra for the 835 keV photon of 54Mn. The result is the spectrum of the energy absorbed by the scintillator per emission of an 835 keV gamma ray. This exercise was proposed for a standard 20 ml LS glass vial and for LS cocktail volumes of 10 and 15 ml. The calculation was done for two different cocktails: toluene and a widely used commercial cocktail, Ultima Gold. The paper describes the results obtained by nine participants using a total of 12 calculation codes.

Absolute activity measurement of the electron-capture-based radionuclides 139Ce, 125I, 192Ir and 65Zn by liquid scintillation coincidence counting.

Four radionuclides with electron-capture-based decay schemes have been directly measured by a liquid scintillation coincidence extrapolation technique. 125I, 192Ir and 65Zn were measured as part of international key comparisons held under the auspices of the International Bureau of Weights and Measures (BIPM). The 139Ce measurements formed part of a regional comparison organized by the Asia Pacific Metrology Programme (APMP). Since 139Ce decays purely by electron-capture, the basic method is described for this radionuclide. Results and difficulties encountered are discussed and uncertainty budgets are presented.

Activity measurements of the high-energy pure beta-emitters 89Sr and 90Y by the TDCR efficiency calculation technique.

The absolute activities of the pure beta-emitters 89Sr and 90Y have been determined by a direct method, namely the triple-to-double coincidence ratio (TDCR) efficiency calculation technique. This undertaking has extended further the number of radionuclides that have been standardized by this non-extrapolation liquid scintillation (LS) method. Both measurements were carried out within the framework of international key comparisons under the auspices of the International Bureau of Weights and Measures (BIPM). The TDCR results agreed well with those of other participating national laboratories, most using alternative (tracer) methods.

The IFIN-HH triple coincidence liquid scintillation counter.

The paper summarizes the IFIN-HH triple coincidence liquid scintillation counter used for the implementation of the TDCR method. The electronic unit was recently extended to record the three individual double coincidence ratios to take into account the differences in the quantum efficiencies of the three-photomultiplier tubes. Some details of the electronic system and the data processing are given. The critical point of a TDCR counter is to adjust correctly the discriminator levels on the three channels under the single electron peak. The paper describes the method of adjustment based on the evolution of the dark counting rate versus the discriminator level. Also indicated is the influence of the discrimination level on the activity results as measured at IFIN-HH using a 3H standard. The performances of the IFIN-HH TDCR counter was checked against the measurement results of the TDCR counters of CSIR NML (South Africa), RC (Poland) and LNHB (France). A set of ready-to-measure 63Ni sources in liquid scintillator, in sealed counting vials, was prepared and dispatched for measurement to all these laboratories. The paper describes designs of the TDCR counters used. An analysis and discussion of the measurement results is given.

The standardization of 33P by the TDCR efficiency calculation technique.

The activity of the pure beta-emitter phosphorus-33 (33P) has been directly determined by the triple-to-double coincidence ratio (TDCR) efficiency calculation technique, thus extending the number of radionuclides that have been standardized by this simple, non-extrapolation liquid scintillation (LS) method. The major advantage of inherently accounting for chemical quenching without the need for additional external measurements is demonstrated. The 33P solution activity concentration was verified by tracing with cobalt-60, utilizing 4pi(LS)beta-gamma coincidence counting. Agreement to within 1.2% confirmed the reliability of the TDCR measurements.

Direct activity determination of 54Mn and 65Zn by a non-extrapolation liquid scintillation method.

The measurement of 54Mn and 65Zn by liquid scintillation coincidence counting results in low detection efficiencies. The activity obtained from the extrapolation of efficiency data can therefore become problematic if curvature is present. The simple decay scheme exhibited by these radionuclides, with the emission of an energetic gamma ray, allows the absolute activity to be determined from 4pie-gamma data by direct calculation without the need for efficiency extrapolation. The method, which relies on determining the probability of the gamma-ray interacting with the scintillator solution, is described and validated by measurements made on 60Co.

Preparation of solid water-equivalent radioactive standards.

The use of a superabsorbent polymer to prepare water-equivalent volume standards by solidification without the need of irradiation to effect the polymerization process, is described. Less than 40 g of the polymer is needed to solidify 1 litre of solution. Monte Carlo simulations of the gamma-ray escape probability indicate that the mixture is water-equivalent to better than 1.0%. During preparation, the solidified material can be mixed until homogeneity is achieved. Comparative measurements made before and after solidification confirmed the homogeneity and demonstrated water equivalence.

Radioactivity standardization in South Africa.

South Africa's national radioactivity measurement standard is maintained at a satellite laboratory in Cape Town by the National Metrology Laboratory (NML) of the Council for Scientific and Industrial Research. Standardizations are undertaken by a number of direct methods utilizing liquid scintillation counting (LSC). The successful application of LSC to the 4pi beta-gamma coincidence method is reviewed. The activity unit is maintained through radionuclide specific calibration factors relating to a pressurized re-entrant well type ionization chamber. A comparison is made between normalized factors given by the manufacturer and deduced factors obtained by a method used to transfer calibration factors from the International Reference System of the International Bureau of Weights and Measures based on the NML's own absolute standardizations.