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The spatial distribution of barium activity in granitic rocks was measured with two autoradiography techniques; digital autoradiography using phosphor imaging plate technique (Fuji 5100) and filmless electronic autoradiography (i.e. The BeaQuant (TM)), which is based on a gas detector incorporated in a micromesh Parallel Ionization Multiplier (PIM). Rock cubes taken from a diffusion experiment that were in contact with Ba-133 tracer were measured to determine diffusion profiles. In addition, the spatial distribution of Ba-133 in the samples was determined. Polymethyl methacrylate standards for Ba-133 were developed to determine the counting efficiency for electronic autoradiography. Good visual correlation between the two autoradiography methods were obtained in this study. The results of the experiments presented here can be utilized in future studies on the diffusion behavior of barium in granitic rocks.

The Fukushima Dai-Ichi Nuclear Power Plant (FDNPP) accident that occurred in March 2011 released significant quantities of radionuclides into the environment. Ten years after the accident, questions still remain, particularly about the processes that led to the partial core meltdown of reactors 1 and 3. So far, some answers have been provided by the investigation of particles containing caesium (Martin et al., 2020) and sometimes uranium (Ochiai et al., 2018). Indeed, the composition of particles, which were produced and spread at the time of the reactor explosion, reflect the conditions that prevailed in the reactor. Accordingly, the objective of the current research is to develop a method for specifically locating actinide-bearing particles in sediment samples collected in the vicinity of FDNPP. To identify and locate such particles, three already existing methods have been upgraded, including 1) the method of fission tracks already used in the field of non-proliferation studies, 2) the autoradiography through the use of imaging plates that are currently employed in the context of the localization of particles containing radio-caesium and the dismantling of nuclear facilities (Haudebourg and Fichet, 2016), and 3) a real time autoradiography method through the use of the BeaQuant® instrument which has been developed for detecting radioactive particles in biology and geosciences.In this study, a sediment sample collected nearby FDNPP, which may contain particles containing both radio-caesium and actinides, was selected. This sample was dried and sieved to 63 µm before being processed according to the different analysis protocols. A quality control sample containing only uranium oxide particles was also analysed, as these particles are devoid of gamma-emitters.The first results of this comparison of autoradiography methods for the detection of actinide-bearing particles in Fukushima samples will be presented. The method of fission tracks was particularly efficient for detecting both natural and anthropogenic uranium.The next steps of this study will be to implement this method identified as optimal to isolate and characterise a larger number of particles released by FDNPP. The full characterization of these particles (size, morphology, elemental and isotopic compositions) will provide novel insights to determine their origin and to improve our understanding of their formation processes within the reactors and anticipate their fate in the environment.References:Haudebourg, R., Fichet, P., 2016. A non-destructive and on-site digital autoradiography-based tool to identify contaminating radionuclide in nuclear wastes and facilities to be dismantled. J. Radioanal. Nucl. Chem. 309, 551–561. https://doi.org/10.1007/s10967-015-4610-7Martin, P.G., Jones, C.P., Cipiccia, S., Batey, D.J., Hallam, K.R., Satou, Y., Griffiths, I., Rau, C., Richards, D.A., Sueki, K., Ishii, T., Scott, T.B., 2020. Compositional and structural analysis of Fukushima-derived particulates using high-resolution x-ray imaging and synchrotron characterisation techniques. Sci. Rep. 10, 1636. https://doi.org/10.1038/s41598-020-58545-yOchiai, A., Imoto, J., Suetake, M., Komiya, T., Furuki, G., Ikehara, R., Yamasaki, S., Law, G.T.W., Ohnuki, T., Grambow, B., Ewing, R.C., Utsunomiya, S., 2018. Uranium Dioxides and Debris Fragments Released to the Environment with Cesium-Rich Microparticles from the Fukushima Daiichi Nuclear Power Plant. Environ. Sci. Technol. 52, 2586–2594. https://doi.org/10.1021/acs.est.7b06309

International audience; A new approach is proposed in order to spatially localize and determine the equilibrium state of natural decay chains on hand-scale geological samples, thanks to a combination of three techniques: 1) Elementary chemical mapping by microprobe; 2) Alpha autoradiograph by gaseous detectors and 3) bulk alpha particle spectrometry. The quantitative nature of alpha autoradiograph and its comparison with U chemical maps allows to locate radioactive equilibrium state in four samples. This equilibrium state was confirmed by alpha spectrometry analysis.

In Finland and Sweden the KBS-3 concept has been chosen for the disposal of spent nuclear fuel in crystalline rock. Recent experiments have shown that heterogeneity of rock may play a major role in the transport of radionuclides. Autoradiographic methods have been proven to be able to assist the characterization of heterogeneous structures. In this study we tested a novel filmless autoradiographic device called BeaverTM which applies a micro patterned gaseous detector in order to quantitatively map beta emissions from C-14 atoms. The studied samples were impregnated with C-14-labelled methylmethacrylate (C-14-MMA) and polymerized to C-14-PMMA with thermal initiator. The BeaverTM was then used to determine the spatial distribution of the C-14-PMMA by measuring the C-14 emissions. The porosity is determined from the amount of C-14-PMMA in the rock sample and results were compared to ones from phosphor imaging plate autoradiography. The resulting images show a heterogeneous distribution of porosity which arises from the different minerals. The samples were chosen from three sites that have been used recently for in situ diffusion experiments: Olkiluoto (Finland), Aspo (Sweden) and Grimsel (Switzerland).

International audience

The spatial distribution of barium activity in granitic rocks was measured with two autoradiography techniques; digital autoradiography using phosphor imaging plate technique (Fuji 5100) and filmless electronic autoradiography (i.e. The BeaQuant™), which is based on a gas detector incorporated in a micromesh Parallel Ionization Multiplier (PIM). Rock cubes taken from a diffusion experiment that were in contact with

A new approach is proposed in order to spatially localize and determine the equilibrium state of natural decay chains on hand-scale geological samples, thanks to a combination of three techniques: 1) Elementary chemical mapping by microprobe; 2) Alpha autoradiograph by gaseous detectors and 3) bulk alpha particle spectrometry. The quantitative nature of alpha autoradiograph and its comparison with U chemical maps allows to locate radioactive equilibrium state in four samples. This equilibrium state was confirmed by alpha spectrometry analysis.

International audience; In rocks or artificial geo-materials, radioactive isotopes emitting alpha particles are dispersed according to the mineralogy. At hand specimen scale, the achievement of quantitative chemical mapping of these isotopes takes on a specific importance. Knowledge of the distribution of the uranium and thorium series radionuclides is of prime interest to several disciplines, from the geochemistry of uranium deposits, to the dispersion of uranium mill tailings in the biosphere. The disequilibrium of these disintegration chains is also commonly used for dating. However, some prime importance isotopes, such as 226Ra, are complicated to localize in geo-materials. Because of its high specific activity, 226Ra is found in very low concentrations (~ppq), preventing its accurate localization in rock forming minerals.This paper formulates a quantitative answer to the following question: at hand specimen scale, how can alpha emitters in geo-materials be mapped quantitatively? In this study, we tested a new digital autoradiographic method (called the Beaver™) based on a Micro Patterned Gaseous Detector (MPGD) in order to quantitatively map alpha emission at the centimeter scale rock section. Firstly, for two thin sections containing U-bearing minerals at secular equilibrium, we compared the experimental and theoretical alpha count rates, measured by the Beaver™ and calculated from the uranium content, respectively. We found that they are very similar. Secondly, for a set of eight homemade standards made up of a mixture of inactive sand and low-radioactivity mud, we compared the count rates obtained by the Beaver™ and by an alpha spectrometer. The results indicate (i) a linearity between both count rates, and (ii) that the count obtained by the Beaver™ can be estimated from the count obtained by the alpha spectrometry using a factor of 0.82.

Gaseous PhotoMultipliers (GPM) are a very promising alternative of vacuum PMTs especially for large-size noble-liquid detectors in the field of Functional Nuclear Medical Imaging and Direct Dark Matter Detection. We present recent characterization results of a Hybrid-GPM made of three Micropattern Gaseous Structures; a Thick Gaseous Electron Multiplier (THGEM), a Parallel Ionization Multiplier (PIM) and a MICROMesh GAseous Structure (MICROMEGAS),operating in Ne/CF4 (90:10). Gain values close to 10^7 were recorded in this mixture, with 5.9keV x-rays at 1100 mbar, both at room temperature and at that of liquid xenon (T = 171K). The results are discussed in term of scintillation detection. While the present multiplier was investigated without photocathode, complementary results of photoextraction from CsI UV photocathodes are presented in Ne/CH4 (95:5) and CH4 in cryogenic conditions., Comment: 7 pages, 6 figures, Proceeding of the NDIP Conference 2011 to be published in NIM A

Liquid xenon (LXe) is a very attractive material as a detection medium for ionization detectors due to its high density, high atomic number, and low energy required to produce electron-ion pairs. Therefore it has been used in several applications, like {\gamma} detection or direct detection of dark matter. Now Subatech is working on the R & D of LXe Compton telescope for 3{\gamma} medical imaging, which can make precise tridimensional localization of a ({\beta}+, {\gamma}) radioisotope emitter. The diffusion of charge carriers will directly affect the spatial resolution of LXe ionization signal. We will report how we measure the transverse diffusion coefficient for different electric field (0.5 ~ 1.2 kV/cm) by observing the spray of charge carriers on drift length varying until 12cm. With very-low-noise front-end electronics and complete Monte-Carlo simulation of the experiment, the values of transverse diffusion coefficient are measured precisely., Comment: 6 pages, 6 figures, proceeding of DSL-2011

Operation results are presented of a UV-sensitive gaseous photomultiplier (GPM) coupled through a MgF2 window to a liquid-xenon scintillator. It consisted of a reflective CsI photocathode deposited on top of a THick Gaseous Electron Multiplier (THGEM); further multiplication stages were either a second THGEM or a Parallel Ionization Multiplier (PIM) followed by a MICROMEsh GAseous Structure (MICROMEGAS). The GPM operated in gas-flow mode with non-condensable gas mixtures. Gains of 10^4 were measured with a CsI-coated double-THGEM detector in Ne/CH4 (95:5), Ne/CF4 (95:5) and Ne/CH4/CF4 (90:5:5), with soft X-rays at 173 K. Scintillation signals induced by alpha particles in liquid xenon were measured here for the first time with a double-THGEM GPM in He/CH4 (92.5:7.5) and a triple-structure THGEM/PIM/MICROMEGAS GPM in Ne/CH4 (90:10) with a fast-current preamplifier., Comment: 12 pages, 9 figures, submitted to JINST