Nuclear materials characterization in 870 L cemented waste drums is challenging due to significant neutron and gamma ray attenuation. Among the existing non-destructive approaches, photon active interrogation is of particular interest. A LINAC accelerates electrons to energies greater than 10 MeV, leading to highly penetrating interrogating bremsstrahlung photons that can reach nuclear materials in the depth of the 870 L waste drum and allow the detection of delayed gamma rays emitted by photofission products. Because the interrogating photon and neutron fluxes are extremely high during irradiation, measurements with high purity germanium detectors are usually performed after a long irradiation time, for example by moving the detector or the waste drum. Therefore, such measurements are only sensitive to delayed gamma rays associated to photofission products having sufficient long half-life of at least tens of seconds, which cuts a valuable signal coming from fission products with a shorter half-life. In this paper, we report gamma rays measurements of very short lived photofission products using a 3 in x 3 in cylindrical LaBr3(Ce) fast scintillation detector. A depleted uranium sample was irradiated by a pulsed bremsstrahlung source with maximum energy 17.5 MeV in a macro pulsing mode (1 s irradiation, 2 s cooling). This allowed to acquire a strong delayed gamma signal within a time window of 2 s.A clear signature of nuclear materials was observed even in the depth of a concrete mock-up, with an excellent signal-to-noise ratio beyond 3.5 MeV where the background of nonnuclear activated materials is negligible. These results are compared to a semi analytical model that qualitatively agrees but underestimates the measurements by a constant factor 1.7, probably caused by a wrong beam intensity normalization. Indeed, in this work the LINAC pulse time structure (macro pulsing) was different from its nominal working point used to characterize the beam (usual pulsing mode). Since it allows direct calculations of the detector response to delayed gamma-ray photofission measurements, this model is a fast calculation alternative to time-consuming Monte Carlo simulations, in view of further studies that will follow this feasibility demonstration.
In the frame of a long-term research program on the characterization of large radioactive waste packages by photofission, the Nuclear Measurement Laboratory of CEA IRESNE has measured cumulative yields of Pu-239,U-235 and U-238 photofission products by using a Bremsstrahlung photon beam produced by a 17.5 MeV linear electron accelerator. A characterization of the energy of the Bremsstrahlung photon beam has been carried out by photon activation analysis with different samples of gold, nickel, uranium, zinc and zirconium. The contribution of neutron fission in the different samples has also been estimated by MCNP simulations in order to assess as precisely as possible the photofission yields. Finally, 26 cumulative photofission product yields are reported for Pu-239, 28 for U-238 and 26 for U-235, with half-lives ranging from 14 min to more than 3 days, some of them being not recorded so far in the literature. Among these reported photofission product yields, 18 have been measured for all 3 actinides, which can thus be used for their discrimination. A differentiation criterion based on delayed gamma-ray ratios has been established to determine the most efficient photofission product couples to estimate the enrichment of a U-235/U-238 mixture or the fissile fraction (U-235+Pu-239)/actinide mass in a mixture of uranium and plutonium.
The characterization of radioactive waste packages is mandatory for their transport, interim storage and final disposal. In this framework, the Nuclear Measurement Laboratory of CEA DES IRESNE Institute, at Cadarache, France, uses a high-energy electron linear accelerator (LINAC) to produce an interrogating bremsstrahlung beam with endpoint energies ranging from 9 to 21 MeV to perform X-ray imaging and high-energy photon interrogation on large concrete packages. In particular, highenergy photon beam induces photofission reactions in both fissile ( 235 U, 239 Pu, 241 Pu) and fertile ( 238 U, 240 Pu, 232 Th, etc.) actinides possibly present in the radioactive waste. In order to assess their mass, we use delayed gamma rays emitted by their photofission products, which are measured with a 50 % relative efficiency High-Purity Germanium (HPGe) detector. Actinide differentiation, which is important for the fissile mass estimation, is based on the ratios of gamma rays emitted by different photofission products and requires appropriate corrections for the gamma attenuation in concrete. To this aim, we report here a localization method of point-like nuclear materials in the concrete matrix, based on the differential attenuation of several gamma rays emitted by a same photofission product. We use here the 1435.9 and 2639.6 keV lines of 138 Cs, with both experimental data and MCNP numerical simulations to determine the (r,θ) coordinates of nuclear materials. Then, the depth inside the concrete matrix, which is determined with a precision of a few percent, mainly depending on counting statistics on 1435.9 and 2639.6 keV net peak areas, is used to correct for the different gamma ratios used in the actinide identification method. Experimental tests with uranium samples have been performed to validate the localization method.
In the frame of a long-term research program on the characterization of large radioactive waste packages by photofission, the Nuclear Measurement Laboratory of CEA IRESNE, France, has measured cumulative photofission yields of U-235 and U-238 short-lived and long-lived fission products by using a Bremsstrahlung photon beam produced by a 16 MeV electron linear accelerator (LINAC). To this aim, a characterization of the Bremsstrahlung photon beam has been carried out by photon activation analysis with different samples of gold, nickel, uranium and zirconium. The residual neutron flux exiting the LINAC head (lead collimator, borated polyethylene and cadmium shield) has also been characterized by neutron activation analysis with indium samples to estimate the contribution of photoneutron fissions in the uranium samples used to assess the photofission yields. Finally, 49 fission product yields are reported for U-238 and 26 for U-235, with half-lives ranging from 64 s to more than 3 days, some of them not recorded so far in the literature Some photofission products cumulative yields show significant differences between U-235 and U-238, which confirms the possibility of an isotopic discrimination method based on delayed gamma-ray ratios analysis for radioactive waste characterization.
In the framework of homeland security, the Nuclear Measurements Laboratory of CEA Cadarache is studying the detection of Special Nuclear Materials hidden in sea-going cargo containers. Proof of principle experiments done in the DANAIDES facility of CEA Cadarache shows the feasibility of detecting some dozen of grams of highly enriched uranium by means of neutron interrogation with a 14 MeV D-T pulsed neutron generator and an array of EJ-200 plastic scintillators. We show that uranium can be detected by measuring correlated induced-fission prompt neutrons and gamma rays in coincidence, which is a first attempt with such detectors without neutron-gamma PSD capabilities, or more classically by detecting fission-induced delayed gamma rays.
As part of its R&xD activities in the fields of radioactivewaste drum storage and homeland security, the NuclearMeasurement Laboratory of CEA Cadarache has started studiesrelated to the detection of induced delayed fission gamma rays asa signature of U/Pu presence either in radioactive wastes or incargo containers and luggage. The study described in the presentpaper explores the feasibility of detecting fission delayed gammarays of nuclear materials interrogated by a pulsed neutrongenerator. For this purpose, Monte Carlo simulations have beenperformed with ACT, the MNCP6 Activation Control Card.Simulated results have been compared with experimental data tovalidate the numerical model. Samples of uranium andplutonium have been irradiated for 2 hours with a pulsed D-Tneutron generator delivering 14 MeV neutrons with an averageemission of 8.107 n/s, which are thermalised in a graphite cellcalled REGAIN. At the end of irradiation, activated nuclearmaterials were placed in a low-background, high-resolutiongamma spectroscopy station in order to detect delayed gammarays emitted by fission products. Anomalies have been observedin the calculated time decay curve of fission delayed gamma rayswith MCNP6 ACT card, but the time behavior is correct for non-fission activated materials like aluminum or copper. On the otherhand, the number of counts recorded in the main simulatedgamma ray lines from activated nuclear material fission productsis consistent with the experimental results, thus validating thesimulation scheme in view of further studies on thecharacterization of radioactive waste drums or special nuclearmaterial detection in cargo containers.
The measurement of delayed gamma rays following neutron-induced fission is simulated with MCNP 6.1 to investigate the feasibility of fissile material detection in long-lived, medium activity radioactive waste in 870 L drums. The signal from homogeneously distributed fissile material in the drum is several hundred counts in the main delayed gamma peaks of interest. In a peripheral position or in the drum center, the signal is however too small to allow for a reliable measurement.
The photon interrogation analysis is a nondestructive technique allowing to identify and quantify fissile materials in nuclear waste packages. This paper details an automatic procedure which has been developed to simulate the delayed γ-ray spectra for several actinide photofissions. This calculation tool will be helpful for the fine conception (collimation, shielding, noise background optimizations, etc.) and for the on-line analysis of such a facility.
The underwater Neutron Imaging System to be installed in the Jules Horowitz Reactor (JHR-NIS) is based on a transfer method using a neutron activated beta-emitter like Dysprosium. The information stored in the converter is to be offline transferred on a specific imaging system, still to be defined. Solutions are currently under investigation for the JHR-NIS in order to anticipate the disappearance of radiographic films commonly used in these applications. We report here the performance assessment of Computed Radiography imagers (Imaging Plates) performed at LLB/Orphée (CEA Saclay). Several imaging plate types are studied, in one hand in the configuration involving an intimate contact with an activated dysprosium foil converter: Fuji BAS-TR, Fuji UR-1 and Carestream Flex XL Blue imaging plates, and in the other hand by using a prototypal imaging plate doped with dysprosium and thus not needing any contact with a separate converter foil. The results for these imaging plates are compared with those obtained with gadolinium doped imaging plate used in direct neutron imaging (Fuji BAS-ND). The detection performances of the different imagers are compared regarding resolution and noise. The many advantages of using imaging plates over radiographic films (high sensitivity, linear response, high dynamic range) could palliate its lower intrinsic resolution.
This review paper describes the destructive and non-destructive measurements implemented or under development at CEA, in view to perform the most complete radioactive waste characterization. First, high-energy photon imaging (radiography, tomography) brings essential information on the waste packages, such as density, position and shape of the waste inside the container and in the possible binder, quality of coating and blocking matrices, presence of internal shields or structures, presence of cracks, voids, or other defects in the container or in the matrix, liquids or other forbidden materials, etc. Radiological assessment is then performed using a series of non-destructive techniques such as gamma-ray spectroscopy, which allows characterizing a wide range of radioactive and nuclear materials, passive neutron coincidence counting and active neutron interrogation with the differential die-away technique, or active photon interrogation with high-energy photons (photofission), to measure nuclear materials. Prompt gamma neutron activation analysis (PGNAA) can also be employed to detect toxic chemicals or elements which can greatly influence the above measurements, such as neutron moderators or absorbers. Digital auto-radiography can also be used to detect alpha and beta contaminated waste. These non-destructive assessments can be completed by gas measurements, to quantify the radioactive and radiolysis gas releases, and by destructive examinations such as coring homogeneous waste packages or cutting the heterogeneous ones, in view to perform visual examination and a series of physical, chemical, and radiochemical analyses on samples. These last allow for instance to check the mechanical and containment properties of the package envelop, or of the waste binder, to measure toxic chemicals, to assess the activity of long-lived radionuclides or pure beta emitters, to determine the isotopic composition of nuclear materials, etc.
This paper reports a feasibility study, performed by numerical simulation with MCNPX, of fissile mass characterization in dense, large volume, long-lived and medium activity radioactive waste packages, using photofission delayed gamma rays. High-energy photon interrogation with a 15 MeV LINAC has been modelled for a 1.18 m 3 cemented waste package, coupled to high resolution spectroscopy with a HP Ge detector. The study was carried out by assessing the passive and active backgrounds respectively due to the waste package gamma emission, and to material activation during irradiation, in view to determine the detection limits for the main delayed gamma rays of interest. The obtained detection limits are lower than the expected uranium mass in the waste package. On the other hand, as the photofission signal results from both fissile 235 U and fertile 238 U isotopes, a method for uranium isotopes discrimination based on gamma-ray ratios has been evaluated, showing that photofission delayed gamma rays could be used to assess the fissile mass as well as the total uranium mass.
The feasibility of fissile mass quantification in large, long-lived medium activity radioactive waste packages using photofission delayed gamma rays has been assessed with MCNPX. The detection limit achievable is lower than the expected uranium mass in these waste packages, but the important sensibility to the waste matrix density and sample localization imposes to get an accurate measurement of these parameters. An isotope discrimination method based on gamma-ray ratios has been evaluated showing that photofission delayed gamma rays can be used to measure the fissile mass as well as the total uranium mass.
As part of its R&D programs on non-destructive testing of nuclear waste drums, CEA is commissioning an irradiation cell named CINPHONIE, at Cadarache. This cell allows high-energy imaging (radiography and tomography) on large volumes (up to 5 m 3 ) and heavy weights (up to 5 tons). A demonstrator has been finalized, based on existing components. The X-ray source is a 9 MeV LINAC which produces Bremsstrahlung X-rays (up to 23 Gy/min at 1 meter in the beam axis). The mechanical bench is digitally controlled on three axes (translation, rotation, elevation) and can handle objects up to 2 t. This bench performs trajectories necessary for acquisition of projections (sinograms) according to different geometries: Translation-Rotation, Fan-Beam and Cone-Beam. Two detection systems both developed by CEA-Leti are available. The first one is a large GADOX scintillating screen (800×600 mm 2 ) coupled to a low-noise pixelated camera. The second one is a multi-CdTe semiconductor detector, offering measurements up to 5 decades of attenuation (equivalent to 25 cm of lead or 180 cm of standard concrete). At the end of the acquisition, a Filtered Back Projection-based algorithm is performed. Then, a density slice (fan-beam tomography) or a density volume (cone-beam tomography or helical tomography) is produced and used to examine the waste. Characterization of LINAC, associated detectors as well as the full acquisition chain, are presented. Experimental performances on phantoms and real drum are discussed and expected limits on defect detectability are evaluated by simulation. The final system, designed to handle objects up to 5 tons is then presented.
SICANE is a neutron scattering multidetector facility for the determination of the quenching factor (ratio of the response to nuclear recoils and to electrons) of cryogenic detectors used in direct WIMP searches. Well-collimated monoenergetic neutron beams are obtained with inverse (p,n) reactions. The facility is described, and results obtained for the quenching factors of scintillation in NaI(Tl) and of heat and ionization in Ge are presented.
A possibility to search for elementary particles as dark matter candidates is to detect elastic scattering with cryogenic detectors. For the interpretation of the data one has to determine the detector response to nuclear recoils, the so-called quenching factors. They can differ for the heat-, for the scintillation- and for the ionisation-signal and can be measured by scattering of neutrons. The CRESST- and the EDELWEISS-collaborations have set up a neutron scattering facility for cryogenic detectors at the tandem-accelerator of the Munich 'Maier-Leibniz-Labor'. The scattering angle and the time-of-flight of the neutrons are measured by an array of liquid scintillator cells. The pulsed high energy (11MeV) neutron beam is created by nuclear reaction of a B-11 on a H-2-gas target. The set-up and the results of first tests are presented.
The EDELWEISS Dark Matter search uses low-temperature Ge detectors with heat and ionisation read-out to identify nuclear recoils induced by elastic collisions with WIMPs from the galactic halo. Results from the operation of 70 g and 320 g Ge detectors in the low-background environment of the Modane Underground Laboratory (LSM) are presented.