A compact detector system for simultaneous measurements of the light yield non-linearity and timing properties of scintillators.

This work presents an outline of a detection system that employs the Compton spectrometer method to assess the non-linearity of scintillator light yield. A novel approach is introduced, leading to more accurate measurements through the separate determination of the intrinsic light output parameters and the non-linearity of the scintillators. Key features of this system include the use of a portable scintillation detector with three photomultiplier tubes for precise measurement of the average number of detected photoelectrons and the incorporation of recent advancements in correction techniques for accidental coincidences. The integration of digital acquisition, offline data analysis, and geometric adaptation reduces the time required to perform a measurement. The developed detector can simultaneously measure different timing properties, as well as the relative intensities following ionization excitation in a scintillator. The system's performance is demonstrated through measurements of the light yield dependence on the deposited energy for commercially available liquid, plastic, and inorganic scintillators. Such instrumentation serves as a valuable tool in the development of novel scintillating materials, including liquid or solid organic scintillators, inorganic scintillators, and composite scintillators for electron detection, in addition to traditional X-ray or γ -ray detection.

Uncertainties in TDCR measurement revisited: Contribution of optical effects.

In the Triple to Double Coincidence Ratio method in Liquid Scintillation Counting, the detection efficiency is calculated from the value of a free parameter describing the intrinsic light yield of the counting system. This model is generally based on a Poisson distribution of the number of photoelectrons detected and the detection efficiency is obtained from the complement of the non-detection efficiency. In the classical free parameter model, the mean of the Poisson distribution, m, is a constant but some variability of this mean could be expected from optical effects due to internal reflections inside the LS source or from non-homogeneity of the detection efficiency of the photomultiplier tubes. Then, m becomes a random variable and the distribution of the photoelectrons becomes a compound Poisson distribution, with a random variable as mean value. This paper explores the implications of the variance of m, which were, to our knowledge, never considered previously in the uncertainty budget of TDCR measurements.

Towards a radon-in-water primary standard at LNHB.

Despite widespread radon-in-water measurements, no primary radon-in-water standards currently exist. This work aims to bridge this gap by developing a system to produce radon-in-water reference materials. The system relies on cryogenic, loss-free transfer of radon, which is standardized through defined solid angle measurements, to a radon standard in water. It allows for preparation of liquid scintillation and gamma-ray spectrometry samples with traceable radon-in-water concentrations. The system's design, functionality, and the results of pilot performance tests are described.

The international reference system for beta-particle emitting radionuclides: Validation through the pilot study CCRI(II)-P1.Co-60.

The Bureau International des Poids et Mesures (BIPM) is developing a new transfer instrument to extend its centralized services for assessing the international equivalence of radioactive standards to new radionuclides. A liquid scintillation counter using the triple/double coincidence ratio method is being studied and tested in the CCRI(II)-P1.Co-60 pilot study. The pilot study, involving 13 participating laboratories with primary calibration capabilities, validated the approach against the original international reference system based on ionization chambers, which has been in operation since 1976. The results are in agreement and an accuracy suitable for purpose, below 5×10-4, is achieved. The pilot study also reveals an issue when impurities emitting low-energy electrons are present in the standard solution, which have a different impact on liquid scintillation counting compared to other primary measurement methods.

Impact of the Coarse Indoor Non-radioactive Aerosols on the Background Radon Progenies' Compensation of a Continuous Air Monitor.

ABSTRACT: This paper addresses the problem of false positive alarm when using a continuous air monitor (CAM) in decommissioning sites of nuclear facilities. CAMs are used to measure airborne activity and play an important role in the radiation protection of workers likely to be exposed to radioactive aerosols. Monitors usually sample aerosols on a membrane filter. Radioactive particles sampled are detected through the alpha and beta decays that they emit. These latter ionizing particles are measured online by spectrometry thanks to a Passivated Implanted Planar Silicon detector (PIPS). Alpha and beta decays, in this context, come mainly from the natural radon progeny (218Po, 214Pb, and so on) and, in the case of radioactive contamination, also from artificial radionuclides such as 239Pu or 137Cs. The aim of the CAM is to alert the workers when the artificial airborne activity occurs, always considering the presence of a variable background due to the natural particulate airborne activity. The CAM-specific algorithm considers this background dynamically and continuously, often by using a constant parameter. However, non-radioactive aerosols are also sampled on the membrane filter. These latter make the discrimination more difficult as they lead to the deterioration of the alpha-energy spectrum. In this paper, the effect of coarse non-radioactive aerosols on the CAM response is highlighted with four aerosol size-distributions. The evolution of the background is characterized as a function of the aerosol mass sampled, with the example of a simple algorithm. Thus, in this paper, results show a positive correlation of the background with the aerosol mass sampled by the CAM. In addition, results highlight at least two different evolutionary trends according to the aerosol size distribution. An explanation of these evolutions is given by considering the penetration profile of the natural radioactive aerosols in the granular deposit above the CAM filter. The main consequence of these results is that the background could not be considered as proportional to radon progeny as it is currently used.

Time-domain based evaluation of detection efficiency in liquid scintillation counting.

This work explores the distribution of time intervals between signals from the photomultiplier tubes (PMTs) of a liquid scintillation counting (LSC) system when a scintillation burst caused by an ionizing particle is detected. This distribution is termed the cross-correlation distribution and it is shown that it contains information about the probability to detect a scintillation event. A theoretical model that describes the cross-correlation distribution is derived. The model can be used to estimate the mean number of detected photons in a LSC measurement, which allows the calculation of the detection efficiency. The theoretical findings are validated by Monte Carlo simulations and by experiments with low-energy beta-emitting and electron-capture radionuclides ([Formula: see text], [Formula: see text], [Formula: see text] and [Formula: see text]), with dedicated LSC systems and several commercial LSC cocktails. The results show that some of the parameters of the cross-correlation distribution such as the peak height or the kurtosis can be used as detection efficiency estimators or quenching indicators in LSC. Thus, although the time domain and the cross-correlation distribution have received little to no attention in the practice of LSC, they have the capacity to bring significant improvements in almost all LSC applications related to activity determination of low-energy beta-emitting and electron-capture radionuclides. The results also suggest concepts for the development of innovative LSC systems.

Measurement of the half-life of excited nuclear states using liquid scintillation counting.

This work presents measurements of the half-lives of excited nuclear states of 237Np and 57Fe using a liquid scintillation (LS) spectrometer and a gamma detector. A novel approach for the determination of the half-lives of some excited states is presented which uses only LS counting data from a detector with two PMTs. The lifetime of the 1st and 2nd excited states of 57Fe were obtained without the use of a gamma detector. The obtained value for the 59.54 keV level of 237Np is 67.60(25) ns. The obtained values for the 14.4 keV and 136.5 keV levels of 57Fe are 97.90(40) ns and 8.780(36) ns, respectively. The half-life results from this study are consistent with the average value found in the reference decay data tables and have a lower uncertainty.

On the photomultiplier-tube asymmetry in TDCR systems.

The responses of the three photomultiplier tubes (PMTs) in a triple-to-double coincidence ratio (TDCR) liquid scintillation (LS) system are often not identical. Such asymmetries can have a significant influence on activity determinations. The problem is often solved by means of a minimization algorithm which can easily be applied when analytical methods are used for the efficiency calculation, as is usually done for pure beta emitters. However, for radionuclides with more complex decay schemes, the counting efficiencies are often calculated with stochastic methods and the computation of the required corrections becomes very challenging. This paper presents a new numerical method to overcome the asymmetry problem for such complex decays and a comprehensive study on 55Fe is described in detail. For the measurements, the asymmetry was varied by means of grey filter films which were placed in front of one of the photomultiplier tubes. In the case of the pure electron-capture (EC) radionuclide 55Fe, the asymmetry can also be taken into account with a very simple correction which is derived assuming monoenergetic emissions. This work is also of great importance for the planned extension of the International Reference System (SIR) at the BIPM which will be used for international comparisons in radionuclide metrology.

TRITIUM ANALYSIS IN URINE BY THE TRIPLE-TO-DOUBLE COINCIDENCE RATIO METHOD WITH THE HIDEX 300 SL LIQUID SCINTILLATION COUNTER.

The triple-to-double coincidence ratio (TDCR) method is a liquid scintillation primary method for the absolute activity measurement of pure ß- and pure electron capture emitters. This method requires specific three-photomultiplier liquid scintillation counters. The aim of the present work is to assess the TDCR method performance for routine tritium analysis in urine using an HIDEX 300 SL, the only three-photomultiplier liquid scintillation counter designed for routine laboratories. The physical parameters and the semi-empirical Birks parameter (kB) of the prepared liquid scintillation source were firstly determined. TDCR model equations solving and detection efficiencies calculations for measured samples were performed by TDCR07c computing program. Accuracy, uncertainties and detection limit of TDCR method were assessed through the tritium analysis of six intercomparison urine samples. The results demonstrate that the analytical performance of the TDCR method implemented on the HIDEX 300 SL is conform to the recommendations for the monitoring of workers exposed to tritium.

Half-life determination and comparison of activity standards of 231Pa.

The results of an international comparison of activity measurements of a solution of 231Pa are reported and analysed. Prior to this, no known standardisation of 231Pa by activity measurement had been carried out. The comparison was run in 2017-2018 involving eight laboratories, and returned results with no identifiable inconsistencies between methods or laboratories. The results, including one mass determination, gave a231Pa activity concentration of 41.461(48) kBq g-1 and a231Pa atom concentration of 61.48(23) × 1015 atoms g-1, from which a half-life value of 32 570(130) years was derived.

Simulation of the response of an ionization chamber to 214Bi emission. Application to the measurement of 222Rn.

PENELOPE simulations of a Vinten ionization chamber (IC) were performed to investigate the influence of the thickness of glass-ampoules used in 222Rn standardization. The simulation reveals a non-negligible variation of the energy deposited in the chamber gas region (which may induce a proportional variation of the measured current) when considering the ß transition emissions of the daughters of 222Rn. This reinforces the idea of using a specialist container (made of metal to preserve the integrity of the container) that would circulate between the metrology laboratories in the context of international comparison exercises using the BIPM international reference system (SIR).

Analysis of computational problems expressing the overall uncertainties: photons, neutrons and electrons.

In the frame of the EU Coordination Action CONRAD (coordinated network for radiation dosimetry), WP4 was dedicated to work on computational dosimetry with an action entitled 'Uncertainty assessment in computational dosimetry: an intercomparison of approaches'. Participants attempted one or more of eight problems. This paper presents the results from problems 4-8-dealing with the overall uncertainty budget estimate; a short overview of each problem is presented together with a discussion of the most significant results and conclusions. The scope of the problems discussed here are: the study of a (137)Cs calibration irradiator; the manganese bath technique; the iron sphere experiment using neutron time-of-flight technique; the energy response of a RADFET detector and finally the sensitivity and uncertainty analysis for the recoil-proton telescope discussed in the companion paper.

Design and Application of High Optical Quality YAG:Ce Nanocrystal-Loaded Silica Aerogels.

The intrinsic properties of silica aerogels make them well suited for applications requiring high surface area. Therefore, the dispersion of functional nanoparticles (NPs) in these highly porous structures gives access to materials for wide range of applications such as catalysis, energy storage or sensing. The last one is particularly interesting if such composites possess good optical quality. Herein, the synthesis of monolithic and transparent silica aerogels highly loaded with Y3Al5O12:Ce nanocrystals (NCs) (up to 50 wt %) is reported. The developed composite aerogels can be impregnated with liquids, contrary to most of existing aerogels, which crack because of the strong capillary forces. Therefore, this system is designed as a novel concept of 3D porous scintillator, using the efficient photoluminescent and scintillating properties of Y3Al5O12:Ce. The investigated fluid containing low-energetic ionizing radiation emitters impregnates the material, which assures the efficient harvesting of radiation because of highly developed surface area. Such composites prove to be efficient new-type detectors of low-energy beta radiation both in liquids and gases.

Results of the CCRI(II)-S12.H-3 supplementary comparison: Comparison of methods for the calculation of the activity and standard uncertainty of a tritiated-water source measured using the LSC-TDCR method.

A comparison of calculations of the activity of a 3H2O liquid scintillation source using the same experimental data set collected at the LNE-LNHB with a triple-to-double coincidence ratio (TDCR) counter was completed. A total of 17 laboratories calculated the activity and standard uncertainty of the LS source using the files with experimental data provided by the LNE-LNHB. The results as well as relevant information on the computation techniques are presented and analysed in this paper. All results are compatible, even if there is a significant dispersion between the reported uncertainties. An output of this comparison is the estimation of the dispersion of TDCR measurement results when measurement conditions are well defined.

The half-life of 129I.

The radionuclide 129I is a long-lived fission product that decays to 129Xe by beta-particle emission. It is an important tracer in geological and biological processes and is considered one of the most important radionuclides to be assessed in studies of global circulation. It is also one of the major contributors to radiation dose from nuclear waste in a deep geological repository. Its half-life has been obtained by a combination of activity and mass concentration measurements in the frame of a cooperation of 6 European metrology institutes. The value obtained for the half-life of 129I is 16.14 (12) × 106 a, in good agreement with recommended data but with a significant improvement in the uncertainty.

A new determination of 79Se half-life.

A new value of (79)Se half-life was determined by the means of inductively coupled plasma mass spectrometry (ICP-MS) and liquid scintillation counting (LSC) on a sample source isolated from a nuclear reprocessing solution. The procedure used to extract Se from the complex sample solution consisted in liquid-liquid extraction and ion exchange chromatographic methods. The concentration of (79)Se was measured using ICP-MS coupled with electro-thermal vaporisation to eliminate potential isobaric interferences. The activity was measured using LSC after gamma-ray spectrometry to check the contribution of residual radioactive contaminants. From these results, the half-life of (79)Se was found to be 3.77 (19) x 10(5) a.

Residual radioactivity of treated green diamonds.

Treated green diamonds can show residual radioactivity, generally due to immersion in radium salts. We report various activity measurements on two radioactive diamonds. The activity was characterized by alpha and gamma ray spectrometry, and the radon emanation was measured by alpha counting of a frozen source. Even when no residual radium contamination can be identified, measurable alpha and high-energy beta emissions could be detected. The potential health impact of radioactive diamonds and their status with regard to the regulatory policy for radioactive products are discussed.

Advancements in NORM metrology - Results and impact of the European joint research project MetroNORM.

The results of the three years European Metrology Research Programme's (EMRP) joint research project 'Metrology for processing materials with high natural radioactivity' (MetroNORM) are presented. In this project, metrologically sound novel instruments and procedures for laboratory and in-situ NORM activity measurements have been developed. Additionally, standard reference materials and sources for traceable calibration and improved decay data of natural radionuclides have been established.

Implementation of the TDCR liquid scintillation method at CNEA-LMR, Argentina.

During the last two years, a triple-to-double coincidence ratio (TDCR) system was assembled and adjusted at the CNEA-LMR, Argentina. The new counting system will add complementary capabilities to the absolute measurements section of the CNEA-LMR. This work describes its implementation and validation. Several checks and a set of beta-emitting standard solutions were used in order to perform the validation experiments. In preliminary measurements, a 3H LNHB solution with reference activity concentration of (119.7+/-0.9) kBq/g on 11 November 2003 was used. The CNEA-LMR TDCR counter gave, at the same reference date, an activity concentration of (120+/-1) kBq/g. Results and improvements are presented in detail. Concerning the asymmetry of the system, the quantum efficiency of the three photomultiplier tubes was studied for different operating conditions of the focusing voltage. The counter also includes an automatic system to change the efficiency by defocusing the photomultipliers and on the other hand, it was coupled to a HPGe detector to also measure beta-gamma coincidences.

Determination of the intensity of X- and gamma-ray emissions in the decay of 153Sm.

The activity of a 153Sm solution was determined by means of liquid scintillation counting and an ionization chamber. Several accurately calibrated X- and gamma-ray spectrometers were used to measure point sources. The use of different detectors results in improvements to the accuracy of the data around 100 keV where the efficiency curve changes significantly. Photon emission intensities have been derived for the main X- and gamma-rays, and the 103-keV emission has a measured intensity of (29.07 (20)) per 100 disintegrations.