System for correlating alpha and gamma spectrometry measurements for in situ radiological characterization of samples - Patents.com

Abstract

The present invention relates to an alignment device for aligning an alpha ray detector, a sample, and a gamma ray detector according to an alignment axis, the sample being intended to be disposed between the two detectors, the device comprising: a mounting base having an upper side and a lower side, at least one portion of the mounting base bounded by the upper side and comprising the alignment axis being made from a material that allows gamma rays to pass therethrough; first and second support means each mounted on the upper side of the mounting base, the first support means comprising a body portion having at least one opening, each opening being parallel to the alignment axis; - a first support means and a second support means, the first support means being intended to support an alpha ray detector and comprising a first element fixed relative to the mounting base and a second element attached to the first element and movable vertically relative to the mounting base; - a stop element forming a lateral abutment, the stop element being intended to place the gamma ray detector against the lateral abutment in the alignment axis, the stop element being attached to the underside of the mounting base.

Description

[Technical field]

[0001] The present invention relates to the field of nuclear instrumentation and measurement for the characterization of radioactive waste. [Background technology]

[0002] Usually, the characterization of radioactive waste is carried out using various non-destructive (without destruction of the sample) and passive (detection of radiation naturally emitted by the sample) methods. This is in particular the case for gamma ray spectrometry and passive neutron counting methods.

[0003] Gamma spectrometry makes it possible to obtain qualitative and quantitative information about gamma-emitting radionuclides. However, gamma spectrometry is not suitable for the identification and quantification of alpha emitters due to the interference of other radionuclides (especially fission products) with the low-intensity peaks of interest, which are generally of low energy. Furthermore, gamma spectrometry measurements, especially of low-energy radiation, are sensitive to the high-density matrix of the waste.

[0004] Passive neutron counting techniques (whether total or coincidence counting) do not provide information about neutron-emitting radionuclides. As an example, in the case of coincidence counting, 240 It is common to determine the equivalent mass of Pu. 244 This type of measurement is not appropriate in the presence of strong neutron emitters due to spontaneous fission such as Cm.

[0005] It is possible to assess the amount of activity of radionuclides that are difficult and even inaccessible to measure by non-destructive measurements by knowing the amount of activity of radioactive tracer elements and by knowing the characteristic typical spectrum of the resulting waste. Therefore, knowledge of the typical spectrum, which represents the quantitative inventory of the different radionuclides present in the sample to be characterized, is essential data that must be reliable in order to determine with sufficient accuracy the amount of activity of all radionuclides present in a package of radioactive waste on the basis of passive non-destructive nuclear measurements and, more specifically, the amount of activity of alpha-emitting radionuclides in order to manage safety-critical risks.

[0006] The determination of a representative spectrum is usually established by carrying out destructive measurements on a given number of samples that are sufficiently representative of the waste package, in particular by carrying out radiochemical analyses on these samples.

[0007] Vacuum chamber alpha spectrometry is a technique often implemented to determine the quantitative inventory of alpha-emitting radionuclides. It is a method developed by the group 239 Pu+ 240 Pu, Group 241 Am+ 238 Pu, and finally 244 It allows fractionation of some groups of transuranium elements, such as Cm. This technique allows isotopic fractionation of radionuclide groups through upstream chemical separation during sample preparation. However, this preparation can reduce the representativeness of the sample, especially through dilution. It is also costly and time-consuming and therefore not compatible with the rates imposed by industrial production.

[0008] Reference [1] proposes a device for controlling air pollution by aerosols emitting alpha particles. Its aim is to allow the fractionation of radon progeny of actinides of interest by alpha spectrometry operating under ambient conditions, i.e. at ambient pressure and temperature (as opposed to laboratory alpha spectrometry, which is performed under vacuum). To overcome the fact that alpha spectrometry under ambient conditions significantly degrades the alpha spectrum obtained, preventing the fractionation, the device described in reference [1] uses a collimation grid to select the least attenuated alpha particles to obtain a usable spectrum. This principle is exploited today in some aerosol beacons.

[0009] By the same principle, reference [2] shows that radionuclides 239 Pu, 241 Am, and 244 describes a mobile device on filters for fractionating Cm. These radionuclides 239 Pu, 241 Am, and 244 Cm are produced by multiple neutron capture of spent fuel. They are therefore more likely to be present than other alpha-emitting radionuclides, especially in radioactive waste from nuclear fuel reprocessing. 238 Can be mixed with Pu. 238 The issue of Pu isotopes is 241 The goal is to emit alpha particles at energies substantially close to those emitted by Am. Nevertheless, the energy resolution of the alpha detectors used is 238 Pu and 241 Am are not sufficiently fine to be quantified separately, so alpha and gamma spectrometry measurements must be correlated.

[0010] Reference [3] describes a system for characterizing aerosols by alpha spectrometry with a PIPS ("Passivated Implanted Planar Silicon") detector and gamma spectrometry with a NaI detector. Although the gamma and alpha spectrometry measurements are performed simultaneously on the sample, the data measured by alpha and gamma spectrometry do not appear to be correlated in a way that allows quantifying the different alpha-emitting radionuclides and thus determining the radionuclide ratios in the sample.

[0011] Reference [4] describes a system for quantifying alpha emitters in contaminated effluents by using several Si / diamond detectors distributed in a system (called a tree) generating several measurement paths. This system allows to improve the quantification of alpha emitters, which can only be considered for the effluent. Summary of the Invention [Problem to be solved by the invention]

[0012] The present invention aims to improve the in situ radiological characterization of objects or surfaces contaminated by alpha-emitters, on the one hand qualitatively by determining the nature of the radionuclides present and on the other hand quantitatively by estimating the radioactive portion of the latter.

[0013] Knowledge of this information is essential in the context of the nuclear industry, in particular for the management of radioactive waste, to control risks related to safety criticality as well as radiological consequences for humans and the environment. [Means for solving the problem]

[0014] This object is achieved by an alignment device for aligning an alpha radiation detector, a sample and a gamma radiation detector according to an alignment axis, the sample being intended to be disposed between the two detectors, the device comprising: a mounting base having an upper surface and a lower surface, at least a portion of the mounting base bounded by the upper surface and the lower surface and including the alignment axis, made from a material that is transparent to gamma radiation; - first and second support means, each mounted on an upper side of the mounting base, - the first support means comprises a body part having at least one opening, each opening opening according to a direction parallel to the alignment axis, optionally coaxial with the alignment axis, and an axial abutment part configured to support the sample in the alignment axis, - a first support means and a second support means, the second support means being intended to support an alpha radiation detector and comprising a first element fixed relative to a mounting base and a second element attached to the first element and movable vertically relative to the mounting base; a stop element forming a lateral abutment, against which the gamma ray detector is intended to be placed in the alignment axis, the stop element being attached to the underside of the mounting base; Equipped with.

[0015] Preferably, the alignment axis is vertical.

[0016] A "material that allows the passage of gamma rays" should be understood to be a material that allows the passage of at least 75% of the photon flux with a given energy. In general, this consists of materials with low atomic number, low volumetric mass and low thickness. For example, a 5 mm thick polymethylmethacrylate (PMMA) (1.19 g cm -3 and average atomic number of 6.56) will allow 89% of the 59 keV photon flux to pass at normal incidence on the wall.

[0017] Some preferred but non-limiting aspects of this device are as follows: the stop element is a body part having a half-moon shape extending longitudinally according to the direction of the alignment axis and having a center coaxial with the alignment axis according to a cross section, - the body of the stop element includes at least one notch configured to receive a tray forming the screen and hold the tray parallel to the lower surface of the mounting base; - the first element of the second support means is a frame and the second element of the second support means comprises a shaft fixedly mounted on the first element and a means for holding the alpha radiation detector, e.g. a clamping ring, mounted movably in vertical translation on the shaft, - the body of the first support means is a tray with at least two openings, the first support means further comprising a shaft extending along an axis parallel to and offset with respect to the alignment axis, the tray being rotatably mounted on the shaft, each opening of the tray being capable of facing the alignment axis by rotation of the tray.

[0018] The present invention relates to the same sample containing radionuclides. gamma The present invention also relates to a system for correlating radiation spectrometry measurements with alpha radiation spectrometry measurements, the system comprising: a gamma ray detector capable of performing gamma ray spectrometry measurements; an alpha detector with a collimation grid capable of performing alpha spectrometry measurements; - means for obtaining and analyzing alpha and gamma spectrometry measurements; Equipped with - an alignment device according to the invention configured to align a gamma ray detector, an alpha ray detector and a sample to be measured between the two; - a glove box type containment intended to accommodate the sample and the alpha detector, the mounting base of the alignment device forming all or part of a lower wall of the containment; The present invention is characterized by further comprising:

[0019] Preferably, the containment vessel comprises a number of compartments, which may include a sample packaging compartment and a measurement compartment.

[0020] Advantageously, the system further comprises a collimator intended to be positioned around the gamma detector, said collimator being a tubular body coaxial with the alignment axis, formed by connecting two half-tubes. Preferably, the system further comprises a shelf arranged below the containment vessel, the shelf comprising an opening allowing the passage of the gamma detector and having on its upper side linear guide elements, for example guide rails, associated with each half-tube, allowing to guide each half-tube towards its associated half-tube to form the tubular body of the collimator.

[0021] Finally, the invention relates to a method for determining, by implementation of a system as defined herein above, the amount A(X) of radioactivity of radionuclide X and the amount A(Y) of radioactivity of radionuclide Y emitted by a sample comprising radionuclides comprising radionuclides X and Y, comprising the steps of: - placing the sample within an opening in the body of the first support means; - positioning the alpha detector in an alignment axis relative to the sample by vertical movement of a second element of the second support means; - placing the gamma ray detector in the alignment axis by wedging the gamma ray detector against a lateral abutment of a stop element; - acquiring, preferably simultaneously and during the same counting time, an alpha spectrum and a gamma spectrum; - selecting, in one of the two spectra, an energy line in which the radionuclide X is identifiable and which does not interfere with other radionuclides of the sample, and determining the amount of radioactivity A(X) of the radionuclide X; - selecting an energy line in which only radionuclides X and Y interfere in the other of the two spectra, calculating the contribution of radionuclide X in said line over a number of pulses N(X) and determining the contribution of radionuclide Y in said line over a number of pulses N(Y); - determining the amount of radioactivity A(Y); Includes.

[0022] Since the two measuring devices (alpha and gamma) have their own sensitivity and detection limit, the measurement times of the two measuring devices may therefore be different in order to obtain usable results. The measurements of alpha and gamma radiation do not necessarily have to be performed simultaneously but can be performed successively. What is important is that the measurement geometry is fixed in order to correlate the measurements. The advantage of performing the measurements simultaneously is mainly concerned with the optimization of the measurement times to adapt to the speed imposed by the method.

[0023] According to a first embodiment, the sample is a contaminant present on a sampling surface of a sampling support made from a material that is transparent to gamma rays, and the method preferably further comprises a step of packaging the sample in a compartment of a containment vessel, the packaging step preferably comprising a step of assembling by gluing the sampling surface of the sampling support containing the contaminant with a surface of a protective film, the protective film being made from a material that is transparent to alpha rays, at least in the aperture intended to face the contaminant.

[0024] Preferably, the sampling support is made from polyethylene terephthalate (PET) and includes an adhesive layer on its sampling surface.

[0025] According to another embodiment, the sample is a contaminant present on a sampling surface of a sampling support made of a material transparent to gamma radiation, the method preferably further comprising packaging the sample in a compartment of a containment vessel, the packaging step comprising: - depositing a sample on one side of a planar support made of a material that is transparent to gamma radiation; - assembling by gluing the face of the planar support on which the samples are deposited with the face of a protective film, the protective film being made of a material transparent to alpha radiation, at least in the apertures intended to face the contaminant; Includes.

[0026] Preferably, the surface of the planar support comprises an adhesive layer, which is present prior to deposition of the sample.

[0027] Preferably, the planar support is made from polyethylene terephthalate (PET).

[0028] Advantageously, whether in the first or second embodiment, at least the aperture of the protective film, and preferably the entire protective film, is made from polyethylene terephthalate (PET). Preferably, the aperture of the PET protective film has a thickness of less than or equal to 6 μm.

[0029] A major advantage of the present invention is that the measurements are carried out in situ, without the need for costly and lengthy preparation of samples, as is typically done in laboratories.

[0030] To address the problems of the prior art, the present invention proposes a mobile and portable system, which allows measurements to be carried out at a location closest to the demolition site.

[0031] The system according to the invention comprises a gamma detector (preferably a germanium detector, which allows better performance in terms of energy resolution) and also an alpha detector (preferably a silicon detector, which operates under ambient conditions). Differentiation of alpha emitters under ambient conditions is possible by adding a collimation grid positioned opposite the active surface of the silicon detector. This then makes it possible to detect only the least attenuated alpha particles, which improves the energy resolution and allows the identification of alpha emitters.

[0032] Thanks to the alignment device according to the invention, the alpha and gamma detectors are positioned on the same axis as the axis of the sample. Furthermore, thanks to the alignment device, the measurement geometry is fixed, making it possible to correlate the measurements of alpha and gamma spectrometry, which is necessary to estimate the ratio between different radionuclides (typical spectra).

[0033] The invention will be better understood after reading the following description, given only as a non-limiting example, with reference to the accompanying drawings, in which: [Brief description of the drawings]

[0034] [Figure 1] 1 is a simplified diagram illustrating one embodiment of a correlation system according to the present invention from a side perspective view. [Diagram 2] FIG. 2 is a simplified diagram illustrating another embodiment of a correlation system according to the present invention in a front cross-sectional view. [Diagram 3] FIG. 13 depicts an experimental alpha spectrum performed in the laboratory using an alpha detector with a collimation grid and an electrodeposition source. [Figure 4] FIG. 1 is a top view showing a shelf placed under the glove box and intended to support a collimator of a gamma ray detector. [Diagram 5] 1 is a cross-sectional view illustrating one embodiment of an alignment device according to the present invention. [Figure 6a]FIG. 13 is a cross-sectional front view of a gamma ray detector positioned to strike a stop element. [Figure 6b] FIG. 2 is a cross-sectional view showing a gamma ray detector positioned to strike a stop element. [Figure 6c] FIG. 13 is a side view showing a gamma ray detector positioned to strike a stop element. [Figure 7a] FIG. 1 is a front view of one embodiment of an alignment device according to the present invention. [Figure 7b] 1 is a side view of one embodiment of an alignment device according to the present invention; [Figure 8a] FIG. 13 is a front cross-sectional view of one embodiment showing a screen positioned on a stop element between a gamma ray detector and an underside of a mounting base (not shown). [Figure 8b] FIG. 13 is a cross-sectional view depicting an embodiment showing a screen positioned on a stop element between a gamma ray detector and an underside of a mounting base (not shown). [Figure 8c] FIG. 13 is a side view depicting an embodiment showing a screen positioned on a stop element between a gamma ray detector and an underside of a mounting base (not shown). [Figure 9] 2 is a front (and partial cross-sectional) view of another embodiment of an alignment device according to the present invention; [Figure 10] FIG. 13 is a diagram showing an example of packaging of a sample. [Figure 11] FIG. 1 shows an example of an alpha ray spectrum obtained by simulation by modeling an electrodeposition source. [Figure 12] FIG. 2 shows an example of a simulated gamma ray spectrum. [Figure 13] FIG. 2 is a schematic diagram illustrating the operating principle of the method according to the invention; DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0035] In FIG. 1, a side perspective view of one embodiment of a correlation system 1 according to the present invention is shown.

[0036] In Fig. 2 an embodiment of a correlation system 1 according to the invention is represented in cross section and in front view. In particular, the correlation system 1 comprises a glove box 2, an alpha ray detector 3, a gamma ray detector 4 and an alignment device 5 making it possible to align a sample 6 with the alpha ray detector and the gamma ray detector. It should be noted that in Fig. 2 the second support means 21 of the alignment device 5 are not represented in order to facilitate the reading of the figure.

[0037] The glove box 2 is mobile (transportable) so that it can be positioned closest to the demolition site. This makes it possible to ensure that no contaminants are scattered during the analysis of the samples. It is intended to house the samples 6 to be analyzed, as well as the alpha detector 3.

[0038] Preferably, the glove box 2 is divided into compartments. According to a preferred embodiment, the glove box comprises three juxtaposed compartments (FIG. 2). The first compartment A is used for receiving the sample 6 to be analyzed and packaging it (e.g. shrink-wrapping it). The second compartment B is used for measuring the sample by alpha spectrometry. The third compartment C is used for equipment maintenance (in particular decontamination of the elements of the alpha spectrometry chain).

[0039] Compartment B may also be instrumented with other measuring devices such as: - beta spectrometry detectors for measuring pure beta emitting radionuclides not measurable by alpha and gamma spectrometry; - Total alpha counting probe, - Total beta counting probe.

[0040] Additional compartments may be added if necessary. For example, it is possible to add an airlock between compartments A and B. Indeed, since compartment A is the compartment most likely to be contaminated since the packaging of the sample takes place, by adding an additional compartment between compartments A and B (acting as a transition airlock), excessive contamination of compartment B during the transfer of the sample packaged in compartment A can be avoided.

[0041] Each of the alpha and gamma ray detectors is connected to data acquisition and analysis means 7, such as a multi-channel analyzer and a computer (Figure 1), providing that the computer may be common to both detectors.

[0042] In a known manner, the alpha detector 3 may be associated, by means of a connector, with a preamplifier that allows to collect the charges generated in the detector in order to form a signal whose integral is proportional to the deposited energy, the whole being housed in a protective case that is opaque to visible light and to alpha radiation and has an open cavity that is closed by a collimation grid that is placed near and opposite the entrance aperture (also called active aperture) of the alpha detector. For example, the collimation grid is made of stainless steel. The collimation grid can be replaced in case of contamination. The protective case may then be made of stainless steel.

[0043] The alpha detector 3 is adapted for measuring alpha radiation under ambient conditions. Preferably, it is a silicon detector, such as a PIPS (short for "Passivated Implanted Planar Silicon") detector or a TCAM detector (an extension of the standard CAM detector) from MIRION Technologies. To allow possible decontamination of the alpha detector 3, the entrance aperture of the alpha detector is protected with a layer of varnish.

[0044] The alpha detector 3 operating under ambient conditions has a performance in terms of separating alpha-emitting radionuclides that is substantially equivalent to the performance of a similar alpha detector operating in a vacuum chamber with electrodeposition sources. In particular, it is capable of separating uranium from plutonium, and also radon progeny such as polonium from actinides of interest (Pu, Am, Cm), and also, for example, from groups 239 Pu+ 240 Pu, Group 238 Pu+ 241 Am, and finally 244 A group of Cm radionuclides can be separated.

[0045] The collimation grid of the alpha detector can be sized by simulation to obtain performance similar to that obtained with the alpha detector in the vacuum chamber without upstream isotope separation. The performance of such sized collimator grids has been tested in the laboratory with electrodeposited sources. The performance in terms of energy resolution is given by: 239 Pu, 241 Am, and 244 This is the alpha peak of Cm at 70 keV to 80 keV (Figure 3). Recall that when we refer to energy resolution, we are talking about the half-height width of the alpha peak. Note that at a resolution of 70 keV to 80 keV, it is possible to resolve the peaks.

[0046] As illustrated in FIGS. 1 and 2, the gamma ray detector 4 is located outside the glove box 2 .

[0047] Preferably, the gamma ray detector is a high purity germanium detector. In a known manner, the germanium detectors used in gamma ray spectrometry are of high purity. High purity germanium detectors are currently the most popular detectors in terms of energy resolution, making it possible to identify peaks of interest in the gamma ray spectrum.

[0048] Preferably, the gamma ray detector is a planar detector. Planar detectors are specialized for measuring low to medium energy gamma rays due to their thickness, which is beneficial in our case since the energy rays of the radionuclides of interest are mainly emitted at low energies. The low average value and high energy efficiency allow for a high degree of detection of fission products (e.g. 137 Cs) and activation products (e.g. 60 This is useful in limiting the influence of parasitic radionuclides such as 1Co, which may drown out peaks of interest in their Compton background.

[0049] Due to the nature of the radionuclides present in the contaminants, coincidence effects can occur in gamma measurements. Coincidences are reflected by the simultaneous detection of two or more cascaded gamma photons, which produces a sum peak (which, as the name suggests, is the result of the summation of several peaks) and the result is an over- or under-estimation of the counts in the full energy peak.

[0050] To best overcome this phenomenon, the gamma ray detector 4 is placed at a minimum distance of 10 cm from the sample 6 .

[0051] Planar gamma ray detector 241 The performance of Am identification and quantification was evaluated in the laboratory by numerical simulation. Therefore, the laboratory test was performed using the LEGe™ flat panel detector of MIRION Technology. 137 In the Cs Compton continuum background 241 This was carried out to validate the feasibility of quantifying Am.

[0052] The Am / Cs ratio with a penalty of 0.01 was chosen to examine the extreme and penalizing cases. This ratio corresponds to a radioactive material with an activity of 43,604 Bq. 241 A point source of Am was placed 155 cm from the LEGe™ detector and had a radioactivity of 296,043 Bq. 137 It is experimentally represented by placing a Cs point source 40 cm from the detector.

[0053] In this configuration, 241 It has been shown that it was possible to identify the 59 keV photopeak of Am, and that the uncertainty regarding the number of pulses at this peak reached 10% over a 30 min acquisition.

[0054] To limit the ambient background noise during the acquisition of the gamma ray spectrum (i.e. radionuclides naturally present in the surrounding material, cosmic rays, and even all parasitic radiation emitted by radioactive sources located outside the collimator's field), a lead shield is placed around the gamma ray detector and the stop elements of the alignment device. This shield also serves as a collimator 8 through the reduction of the solid angle of the gamma ray detector 4 relative to the dimensions of the sample 6. Furthermore, the collimator 8 can be covered on its inner walls with a copper sheath 9 to attenuate the lead X-rays that degrade the low-energy gamma ray spectrum. This shield makes it possible to avoid saturating the electronics of the gamma ray detector with parasitic radiation.

[0055] There are different possibilities for placing the collimator 8 around the gamma detector and the stop element, but what is important is to place the collimator to accommodate the configuration of the glove box (space available under the glove box) and the dimensions of the gamma detector. For example, as illustrated in FIG. 2, the collimator 8 can be positioned on a shelf 10 that is located below the glove box. The shelf further has an opening 11 (e.g. a groove) sized to allow the passage of the gamma detector. Here, the groove is sized to allow the passage of a rod of a lifting means in which the gamma detector is positioned. This lifting means makes it possible to adjust the distance between the gamma detector and the lower surface of the mounting base 15 (the outer surface of the lower wall of the glove box).

[0056] According to a possible configuration illustrated in FIG. 4, the collimator is divided into two parts 8′ and 8″ (half tubes) which slide along rails 12 present on the shelves so as to form the collimator once joined. Steps 13 present on the side walls of the two parts 8′ and 8″ of the collimator ensure a complete closure of the collimator and therefore an attenuation of the ambient radiation when the collimator is closed, and therefore a radiation protection of the gamma detector. Preferably, the rails 12 are sized such that the collimator is considered closed when the two parts 8′ and 8″ of the collimator abut against the respective rails. According to a variant, a handle can be added to the outer surface of each collimator part 8′ and 8″ to facilitate its movement on the rails 12.

[0057] It is also possible to use a cooler 35, which ensures cooling of the gamma detector during operation. If the gamma detector is a high purity germanium detector, it is possible to use either Dewar cooling with liquid nitrogen or an electrical cooler for cooling the germanium detector.

[0058] The alignment device 5 is a key element of the combination of the information acquired by the two alpha and gamma detectors. Indeed, as already shown, it makes it possible to align the alpha detector / sample / gamma detector set according to an alignment axis 14 and to control the measurement geometry in order to guarantee the reproducibility of the measurements.

[0059] The alignment device 5 includes a mounting base 15 having an upper side and a lower side (FIGS. 5 and 9). At least one portion 16 of the mounting base 15, bounded by the upper side and the lower side and including the alignment axis 14, is made from a material that allows gamma radiation to pass. The entire mounting base may be made from a material that allows gamma radiation to pass. Preferably, the mounting base corresponds to a lower wall of the glove box. If the portion 16 does not correspond to the entire lower wall of the glove box, care will be taken to ensure a seal between the mounting base and the lower wall of the glove box to ensure containment of the glove box.

[0060] The mounting base has at least a portion of a material that transmits gamma rays so that gamma rays emitted from a sample placed inside the glove box can reach the gamma ray detector 4 placed outside the glove box without excessive attenuation of the gamma ray flux. The material that transmits gamma rays is a material that has a low atomic number, a small volumetric mass, and a small thickness. For example, a 5 mm thick polymethyl methacrylate (PMMA) (1.19 g cm -3 A wall with a volume mass of 1.0 and mean atomic number of 6.56 will allow 89% of the 59 keV photon flux to pass at normal incidence on the wall.

[0061] It should also be noted that due to the presence of fissile material in the sample, the parts of the alignment device that are located inside the glove box (the mounting base as well as the first and second support means) cannot be made of PVC (polyvinyl chloride) type material in order to avoid reactions on light nuclei such as chlorine (alpha, n) that generate neutrons.

[0062] The alignment device 5 also comprises a first support means 17 and a second support means 21 each mounted on an upper side of the mounting base 15 .

[0063] The first support means 17 serve to support the sample. They comprise a body 18 with at least one opening 19, each opening opening according to a direction parallel to the alignment axis, possibly coaxial therewith. Each opening also comprises an axial abutment 20, which is adapted to support the sample 6 in the alignment axis 14.

[0064] 5, the body portion 18 may include a single through opening, which is coaxial with the alignment axis 14. Because the opening is open, only the mounting base is between the sample and the gamma ray detector at the alignment axis.

[0065] The second support means 21 serves to support and center the alpha detector 3 in the alignment axis. As illustrated in Fig. 7, the second support means 21 comprises a first element 22 (typically fixed on the mounting base) fixed relative to the mounting base 15 and a second element 23 mounted on the first element 22 and movable vertically relative to said mounting base 15, for holding the alpha detector. As illustrated in Fig. 7, the first element 22 may be a frame and the second element 23 may comprise a shaft 27 fixedly mounted on the first element 22 and a means 28, for example a clamping ring, for holding the alpha detector, which is mounted movable in vertical translation on the shaft 27. The first element 22 is fixed such that the alpha detector is in the alignment axis (and therefore aligned with the sample). The alpha detector 3 is held by a clamp ring and can be positioned in contact or quasi-contact with the sample by being moved vertically with vertical translation of the clamp ring on shaft 27 .

[0066] The alignment device 5 also comprises a stop element 24 forming a lateral abutment, against which the gamma ray detector 4 is intended to be placed in the alignment axis. This stop element is mounted on the underside of the mounting base 15. The gamma ray detector is placed in a position against the stop element 24 so as to be aligned with the sample 6 and the alpha ray detector 3. Figures 6a to 6c show various views of the arrangement of the gamma ray detector against the stop element.

[0067] After the gamma detector is placed, a collimator 8 is placed around the gamma detector and the stop element.

[0068] It is possible to insert one or more screens 26 of different materials and thicknesses between the gamma detector and the sample outside the glove box to adjust the fluence of the low energy gamma photons. One or more notches 25 formed in the stop element 24 allow the positioning of these screens. Figures 8a-c represent examples of positioning a screen on the stop element from different perspectives. For example, the screen may consist of a screen made of cadmium or zinc.

[0069] especially, 241 The use of the screen 26 is necessary when Am is present in large amounts in the sample to be analyzed. In fact, the characteristic line of this radioactive nuclide at 59 keV is very strong. By using a material with a low atomic number (such as cadmium or zinc) and a screen with a thickness that can vary from one to several millimeters, it is possible to attenuate this line at 59 keV and avoid attenuating the lines of higher energy, in order to avoid saturation of the electronics of the gamma ray detector. For example, zinc (atomic number 30, volume mass 7.13 g.cm -3 ) thickness of 2 mm allows attenuating more than 90% of the 59 keV photon flux at normal incidence on this screen.

[0070] especially, 137The screen can accommodate any kind of Am / Cs ratio where americium is very abundant compared to cesium so that Cs can be quantified.

[0071] If the measurement compartment B of the glove box contains different measurement devices, it is interesting to adapt the body 18 of the first support means 17 so that the measurement of the sample 6 can be performed without having to manually transfer the sample 6 from one measurement device to the other. For this purpose, as illustrated in FIG. 9, the first support means 17 is made independent of the mounting base 15. For example, the body 18 is a tray with at least two openings 19, the first support means 17 further comprises a shaft 29 extending along an axis parallel and offset to the alignment axis 14, the tray being rotatably mounted on the shaft, and each opening of the tray may be placed on the opposite side of the alignment axis by rotation of the tray. In FIG. 9, as in the case of the alpha radiation detector 3, the other measurement device 33 is held above the sample thanks to a support means 34 equivalent to the second support means 21.

[0072] Thus, by rotation of the tray it is possible to pass the sample from one measurement probe to the other. The tray may also contain more than two apertures, for example four apertures each serving to support a sample, and the tray may for example have a shape like a four-leaf clover, each leaf of the clover containing an opening, which allows four samples to be analysed simultaneously by placing one of the four measurement probes above each sample.

[0073] The sample 6 to be analyzed is defined as a contaminant that is collected on a contaminated object using a suitable support. The sample 6 therefore comprises the contaminant and at least a sampling support, typically a plate having two planar main faces, the contaminant being placed on at least one of the two main faces of the support.

[0074] It should first be recalled that in order to carry out reliable measurements using an alpha detector, it is essential to avoid the risk of contamination on the collimation grid and on the active surfaces of the alpha detector, which would interfere with the results of the measurement. In fact, the alpha detector can be decontaminated, but the collimation grid cannot.

[0075] To overcome this shortcoming, several proposals have been considered.

[0076] According to a first proposal, alpha measurements can be carried out directly on the source support (contaminated object). Between each measurement, the alpha detector is decontaminated and the collimation grid is changed. This is one of the simplest methods, but also the most expensive.

[0077] According to the second proposal, as in the first proposal, the measurements are carried out directly on the source support and between each measurement a background noise is formed which is subtracted from the next spectrum. This method is simple but significantly slows down the characterization of the sample and involves more uncertainty regarding the measurement results.

[0078] The drawback of these two proposals is the premature aging of the alpha detectors due to contamination, which ultimately results in a deterioration of the detector's performance (effect on the detector's active area). Alpha detectors must therefore be replaced periodically.

[0079] It is also possible to continue sampling of the contaminant on a suitable support.

[0080] Several sampling methods can be considered: it is possible to proceed with sampling by scraping (smear), performed by the operator (manual) or remotely (teleoperated, robotic), it is also possible to proceed with sampling by suction (on filters), and it is also possible to proceed with sampling by adhesion using an adhesive.

[0081] In the case of collection by scraping or suction, the selection of the support of the sample is essential. In fact, the physicochemical parameters of the support should be adapted so that contaminants do not penetrate deep into the support, in order to avoid excessive self-absorption of alpha particles and thus deterioration of the alpha spectrum. However, even here, the problem of contamination of the alpha detector is not solved.

[0082] In the case of adhesive sampling, the contaminants are attached to the "adhesive", so the choice of adhesive material (physicochemical properties and thickness) is an important criterion. This adhesive inevitably causes self-absorption phenomena, but has the advantage that most of the contaminants remain fixed on the support, unlike scraping or suction methods, where the contaminants remaining on the surface may be too unstable. When sampling by adhesion using an adhesive, the contaminants are fixed on the support, thereby making it possible to reduce unstable contaminants at the sample.

[0083] In order to reduce contamination of the alpha detector in the case of sampling by scraping or suction, or even more so in the case of sampling by adhesion, it is also proposed to use a film to contain the contamination.

[0084] In the laboratory, several types of films have been tested to observe the attenuation of alpha particles in this film. It has been shown that a 6 μm thick PET (polyethylene terephthalate) film makes it possible to protect the alpha spectrometer while still obtaining an acceptable alpha spectrum for analysis (switching from an energy resolution of 70 keV without film to 110 keV with film in the case of electrodeposition sources). It is noted that this type of PET material is usually doped with aluminum (aluminized PET) and is used in alpha counting detectors to protect this detector from ambient light.

[0085] Advantageously, the packaging of the samples can be carried out in compartment (A) of the glove box.

[0086] It should be recalled that a sample is a contaminant present on at least one of the faces of a sampling support. Depending on the sampling method, the sampling support is different, but is always made of a material transparent to gamma radiation, and may be, for example, a filter (suction sampling), a plate with an adhesive surface (manual or remote sampling), etc.

[0087] According to a first configuration, the sample is packaged in a sandwich between two planar supports, at least one of which is either partially made of PET (i.e. has an aperture made of PET with a very small thickness (so that alpha particles can also reach the alpha detector)) or is made entirely of PET. For example, the very small thickness is 6 μm or less. These two planar supports may be of film or sheet type.

[0088] For example, in the configuration illustrated in FIG. 10, the sample is sandwiched between two planar supports, one of which is a protective film. The planar support forming the lower element of the stack is a rigid support and is made of a material that is transparent to gamma radiation (as it is intended to be placed facing the gamma radiation detector). The sample is placed on the upper side of the planar support, which is covered with a protective film, which is intended to be placed facing the alpha radiation detector. In this example, the protective film has a PET aperture of 6 μm thickness, and the remaining part of the protective film is made of a material that is flexible but preferably more rigid than the PET aperture of 6 μm thickness. At least one of the planar support and the protective film has an adhesive surface, which makes it possible to fix these two elements and to seal the sample.

[0089] In the configuration illustrated in Figure 10, this is a protective film with a sticky side on the outside of the PET aperture to seal the sample. The 6 μm thick PET aperture is free of adhesive to avoid additional attenuation.

[0090] The planar support is preferably rigid. This makes it possible to keep the sample as flat as possible and therefore to control the measurement geometry for any sample. The rigid planar support makes it easier for the operator to package it in a glove box and also to place it on the axial abutment 20 of the opening 19 of the body 18 of the first support means 17.

[0091] According to another configuration, the sample (contaminant and sampling support) is sandwiched between two 6 μm thick PET films and sealed by thermal adhesion. If the contaminant is sampled on both sides of the sampling support, the sample can be analyzed by an alpha detector on these two sides after being sandwiched between these two PET films (the opposite side of the alpha detector is not important here). The disadvantage of this configuration is that the set is no longer rigid. Moreover, the 6 μm PET film used alone is difficult to handle. Therefore, additional equipment is needed to heat seal the two PET films around the contaminant to package the sample.

[0092] According to another configuration, since the contaminants are sampled from the sticky side of the rigid sampling support, the packaging of the sample consists in applying a protective film (for example a PET sheet with a thickness of 6 μm) on the sticky side of the sampling support, which makes it possible to capture the contaminants.

[0093] Regardless of the method chosen to package the sample, the dimensions of this packaging are adapted to the geometry of the opening in which the sample is intended to be accommodated and its corresponding axial abutment.

[0094] According to one embodiment, the system according to the invention may further comprise an active shield which, together with the gamma detector, forms an anti-Compton device. The anti-Compton device is an interesting option to reduce the uncertainty in the quantification by gamma spectrometry of radionuclides emitting low energy gamma photons. In fact, by reducing the Compton signal on the top of the gamma spectrum, it is possible to obtain a high-energy gamma photon emission of 59.54 keV radionuclides. 241 It has the effect of lowering the detection limit of radionuclides of interest such as Am.

[0095] For example, an anti-Compton device comprises a germanium detector, a scintillator-type detector surrounding the germanium detector, and a lead shield surrounding the set formed by the two detectors. The presence of the lead shield is necessary because the density of the scintillator is not sufficient to stop the ambient radiation. When a gamma photon interacts in the germanium detector, it can be scattered (this is the so-called Compton scattering). If it escapes from the germanium detector, the scattered photon can be detected by the scintillator. This is then subtracted from the gamma ray spectrum acquired with the germanium detector, reducing the Compton background and improving the quantification of the radionuclides.

[0096] The performance of such anti-Compton devices depends on the detection geometry as well as the scintillator used.

[0097] With regard to the method according to the invention, it is based on the correlation of alpha and gamma spectrometry measurements. More specifically, the method according to the invention is based on the detection of radionuclides which are identifiable and quantifiable either by alpha or gamma spectrometry or both.

[0098] This correlation makes it possible to deduce the ratio between the various radionuclides by solving an equation. The combination (or correlation) of measurements obtained by alpha and gamma spectrometry and the determination of the ratio is possible because the measurements are performed on the same sample with a fixed measurement geometry.

[0099] As explained previously, alpha spectrometry in the context of radionuclide identification can be applied to samples such as uranium / plutonium mixtures, radon actinide / progeny mixtures, etc.

[0100] Examples of samples containing a mixture of radionuclides are referred to herein as being of the group 239 Pu+ 240 Pu, Group 238 Pu+ 241 Am, and actinides 244 Cm, are processed to distinguish between different groups of actinides.

[0101] FIG. 11 is an example of a spectrum that may be acquired by an alpha detector operating under ambient conditions.

[0102] For each radionuclide, the alpha peak represents the sum of the different lines corresponding to each alpha particle emitted by the sample. It is not possible to distinguish the fine structure of each radionuclide, and it is difficult to distinguish between different radionuclides that emit alpha particles at very similar energies (especially on the one hand). 239 Pu and 240 Pu, on the other hand 238 Pu and 241 It is also impossible to distinguish between the two.

[0103] Table 1 below lists the energies of the alpha particles emitted for the alpha ray spectrum of Figure 11.

[0104] [Table 1]

[0105] The aim is to be able to describe these radionuclides individually.

[0106] For example, to quantify plutonium in radioactive waste, 238 Pu and 241 It is important to be able to separate Am.

[0107] of interest in gamma ray spectrometry, 238 Pu and 241 The energy rays involving Am are as follows:

[0108] [Table 2]

[0109] The gamma ray intensity is low and there are many interferences. Only the gamma ray peaks with energies of 59.54 keV and 125.3 keV can be utilized because there is no interference with other radionuclides and the 59.54 keV peak is preferred for intensity considerations.

[0110] An example of a gamma ray spectrum with possible energy line identification is shown in Figure 12. The spectra in Figures 11 and 12 are simulated spectra, and it has been specified that the sample considered is the same in both cases.

[0111] By gamma ray spectrometry 241 Through quantification of Am 238 It is possible to determine the amount of Pu radioactivity by following the steps below. - By gamma ray spectrometry using the 59.54keV gamma ray peak 241 determining the amount of radioactivity of Am; A( 241 Am) = known (1) - Alpha peak ( 241 Am+ 238Pu) 241 Calculating the Am contribution (number of pulses N), N α ( 241 Am)=A( 241 Am) × ε α ( 241 Am)×I α ( 241 Am)×t (2) Here, ε α ( 241 Am) 241 corresponds to the alpha efficiency for the energy emitted by an alpha particle in Am, and I α ( 241 Am) 241 corresponds to the alpha emission intensity of Am and is equal to 1 since alpha particles emitted by the same radionuclide are not fractionated, and t corresponds to the counting time in alpha spectrometry. - On the same peak 238 determining the contribution of Pu (number of pulses N); N α ( 238 Pu)=N α (Total)-N α ( 241 Am) (3) Here, N α (Total) is Alpha Peak 241 Am+ 238 corresponds to the total number of pulses in Pu. - 238 determining the amount of Pu radioactivity; A( 238 Pu)=N α ( 238 Pu) / [ε α ( 238 Pu)×I α ( 238 Pu)×t] (4) Here, ε α ( 238P Pu) is 238 corresponds to the alpha efficiency for the energy emitted by a Pu alpha particle, I α ( 238 Pu) is 238corresponds to the Pu alpha emission intensity, and t corresponds to the counting time in alpha ray spectrometry.

[0112] Therefore, in general, - If two radionuclides X and Y interfere in the alpha spectrum, and radionuclide X is distinguishable and quantifiable by its gamma spectrum, then the amount of radioactivity of Y is

number

number

[0113] Counting time t in alpha spectrometry α and the counting time t of gamma ray spectrometry γ Note that may vary.

[0114] In summary, the steps to be followed for the method according to the invention are illustrated in FIG. 13, where A(X) corresponds to the amount of radioactivity of radionuclide X (in Bq), A(Y) corresponds to the amount of radioactivity of radionuclide Y (in Bq), and N γ (X) corresponds to the number of pulses of the photoelectron peak corresponding to the radionuclide X in the gamma-ray spectrum, and N α (Total)=N α (X)+N α (Y) and N α (X) corresponds to the number of pulses of the alpha peak corresponding to radionuclide X in the alpha spectrum, and N α (Y) corresponds to the number of pulses of the alpha peak corresponding to the radionuclide Y in the alpha spectrum, and ε γ(X) corresponds to the absolute efficiency for the energy of the characteristic photoelectron peak of radionuclide X in gamma-ray spectrometry, and ε α (X) corresponds to the absolute energy efficiency of the characteristic alpha peak of radionuclide X in alpha spectrometry, and ε α (Y) corresponds to the absolute efficiency of the characteristic alpha peak of radionuclide Y in alpha spectrometry with respect to the energy, and I α (X) corresponds to the intensity of the alpha particles emitted by radionuclide X (i.e. 100% since the rays are not fractionated), and I α (Y) corresponds to the intensity of the alpha particles emitted by radionuclide Y (i.e. 100% since the rays are not fractionated), and I γ (Y) corresponds to the intensity of the gamma photons emitted by the radionuclide Y, and t γ corresponds to the counting time in gamma ray spectrometry, and t α corresponds to the counting time in alpha spectrometry.

[0115] The feasibility of the above example has been verified in the laboratory by gamma spectrometry, especially for radionuclides present strongly in radioactive waste. 137 Disappearing into the background of Cs 241 The possibility of detecting and quantifying Am has been verified.

[0116] In nuclear measurements it is common practice to define the concepts of decision threshold (DT) and detection limit (DL).

[0117] in particular, 241 For Am measurements, if the number of pulses at the 59.54 keV peak is higher than the detection limit, 241 Am is quantifiable if the number of pulses is below the detection limit but above the detection threshold. 241 Am is detectable but not quantifiable. If the number of pulses is below the detection threshold, 241 It is not possible to detect Am.

[0118] The detector threshold (DT) and detection limit (DL) are

number

[0119] Peak surface area N net If is higher than DT, N net The uncertainty of

number

[0120] Within 0.01 241 Am / 137 In the context of imposing penalties involving Cs ratios, 241 The 59.54 keV gamma-ray peak of Am allows quantification of this radionuclide, even after 15 minutes of counting (number of pulses > DL).

[0121] The uncertainty of this value depends on the counting time and also on the release of the sample.

[0122] The quality of the binding then depends on several factors, in particular the counting time for gamma and alpha spectrometry and the emission of the sample.

[0123] It should be noted that the uncertainties regarding the amount of radioactivity estimated by gamma spectrometry are even more significant due to the low energy of the gamma photons measured.

[0124] The uncertainties related to the alpha spectrum are then more numerous, especially with regard to the choice of the sample support (choice of film, sampling method, etc.), whose physicochemical parameters influence the degradation of the alpha spectrum. Indeed, the more contaminants penetrate into the source support, the more the alpha spectrum is degraded.

[0125] Finally, control of the detection geometry is a key aspect of the method to limit sources of uncertainty.

[0126] In conclusion, the present invention makes it possible to use interesting applications in nuclear instrumentation and measurement, especially in the fuel cycle field (mainly downstream of the cycle).

[0127] Its first application is the (near) real-time radiological characterization of radioactive waste, which allows to determine the standard spectra (ratio between radionuclides) of each waste package and participates in the selection of the orientation of radioactive waste towards suitable storage locations according to the radioactive material inventory.

[0128] The quantification of alpha-emitting elements is of great importance with regard to risks related to safety criticality. Until now, the measurement techniques currently used either were not even able to quantify and identify these radionuclides (this is especially the case for gamma spectrometry and neutron measurements) or did not allow to obtain results in real time, requiring a long and costly preparation of the sample, as is the case for alpha spectrometry in a laboratory vacuum chamber.

[0129] The method according to the invention makes it possible to obtain a radiological characterization of the waste almost in real time and without having to carry out lengthy and costly sample preparation upstream of the formation of the waste packages, thus making it possible to save time and costs for the characterization of a large number of wastes.

[0130] Furthermore, in the method according to the invention, the measurements can be carried out on-site closest to the demolition site.

[0131] It is noted that the invention may also be applied in other fields, in particular in the field of environmental protection and monitoring (in the event of an accident or in simple control), but also in the defense, medical and educational fields.

[0132] (References) References [1] French Patent No. 2563633, filed on April 27, 1984 Reference [2] Pollanen et al., “In-situ alpha spectrometry from air filters at ambient air pressure”, Radiation Measurements, vol. 53-54, pp. 65-70, 2013 References [3] China Patent No. 104215997, filed on September 3, 2014 References [4] French Patent No. 2965937, filed on October 7, 2010 [Explanation of symbols]

[0133] 1 Correlation System 2 Glove box 3. Alpha ray detector 4. Gamma ray detector 5 Alignment Device 6. Samples 7 Data Acquisition and Analysis Methods 8 Collimator 8' half tube 8'' half tube 9. Sheath 10 Shelves 11 Opening 12 Rail 13 Step section 14 Alignment Axis 15 Mounting base 16 parts 17 First Support Means 18 Main body 19 Opening 20 Axial contact part 21 Second Support Means 22 First Element 23 Second Element 24 Stop Elements 25 notches 26 Screens 27 Shaft 28 Means for holding alpha radiation detectors 29 Shaft 33 Measuring Equipment 34 Support means

Claims

1. A system (1) for correlating gamma and alpha spectrometry measurements of the same sample (6) containing a radioactive nuclide, comprising: a gamma ray detector (4) capable of performing gamma ray spectrometry measurements, an alpha detector (3) equipped with a collimation grid and capable of carrying out alpha spectrometry measurements, - means (7) for obtaining and analysing alpha and gamma spectrometry measurements, Equipped with The system (1) comprises: a collimator (8) intended to be positioned around said gamma ray detector (4), said collimator being a tubular body coaxial with the alignment axis, formed by joining two half-tubes (8', 8''); an alignment device (5) for aligning the alpha detector (3), the sample (6) and the gamma detector (4) according to an alignment axis (14), the sample being intended to be placed between the two detectors, the alignment device comprising: a glove box type containment vessel (2) intended to contain said sample (6) and said alpha detector (3), a mounting base (15) having an upper side and a lower side, at least one portion (16) of said mounting base (15) bounded by said upper side and said lower side and including said alignment axis is made from a material allowing gamma radiation to pass, said mounting base (15) of said alignment device (5) forming all or part of a lower wall of said containment vessel; - first and second support means, each mounted on said upper side of said mounting base (15), said first support means (17) comprise a body (18) having at least one opening (19), each opening opening according to a direction parallel to said alignment axis, possibly coaxial therewith, and comprising an axial abutment (20) adapted to support said sample (6) in said alignment axis (14); - first and second support means (21) intended to support the alpha ray detector (3) and comprising a first element (22) fixed relative to the mounting base (15) and a second element (23) attached to the first element (22) and able to move vertically relative to the mounting base (15); a stop element (24) forming a lateral abutment against which the gamma ray detector (4) is intended to be placed in said alignment axis, said stop element being attached to the lower side of the mounting base (15); an alignment device (5) comprising: The system further comprises:

2. 2. The system of claim 1, wherein the stop element (24) is a body having a half-moon shape extending longitudinally in accordance with the direction of the alignment axis and having a center coaxial with the alignment axis in a cross section.

3. 3. The system of claim 2, wherein the body of the stop element (24) comprises at least one notch (25) configured to receive a tray (26) forming a screen and hold the tray parallel to the lower surface of the mounting base (15).

4. 4. The system according to claim 1, wherein the first element (22) of the second support means (21) is a frame and the second element (23) of the second support means (21) comprises a shaft (27) fixedly mounted on the first element (22) and a means (28) for holding the alpha ray detector, e.g. a clamping ring, mounted movably in vertical translation on the shaft.

5. 5. A system as claimed in any one of claims 1 to 4, wherein the body (18) of the first support means (17) is a tray having at least two openings (19), the first support means (17) further comprising a shaft (29) extending along an axis parallel to and offset with respect to the alignment axis (14), the tray being rotatably mounted on the shaft, and each opening of the tray can be made to face the alignment axis by rotation of the tray.

6. The system according to any one of claims 1 to 5, wherein the containment vessel (2) comprises a plurality of compartments.

7. The system according to any one of claims 1 to 6, further comprising a shelf (10) arranged below the containment vessel (2), the shelf having an opening (11) allowing the passage of the gamma ray detector (4) and having on its upper side linear guide elements (12), e.g. guide rails, associated with each half tube (8', 8''), enabling each half tube to be guided towards its associated half tube to form the tubular body portion of the collimator.

8. A method for determining the amount of radioactivity A(X) of radionuclide X and the amount of radioactivity A(Y) of radionuclide Y emitted by a sample (6) containing radionuclides comprising radionuclides X and Y, by implementing a system (1) according to any one of claims 1 to 7, comprising: - placing said sample (6) in an opening (19) in said body (18) of said first support means (17); - positioning said alpha detector (3) in said alignment axis (14) relative to said sample by vertical movement of said second element (23) of said second support means (21); - placing said gamma ray detector (4) on said alignment axis by wedging said gamma ray detector against said lateral abutments of said stop elements (24); - acquiring an alpha spectrum and a gamma spectrum, preferably simultaneously and within the same counting time; - selecting, in one of the two spectra, an energy ray in which the radionuclide X is identifiable and which does not interfere with other radionuclides of the sample, and determining the amount A(X) of the radioactivity of the radionuclide X; selecting an energy line in which only the radionuclides X and Y interfere in the other of the two spectra, calculating the contribution of the radionuclide X in said energy line over a number of pulses N(X) and determining the contribution of the radionuclide Y in said energy line over a number of pulses N(Y); - determining said amount of radioactivity A(Y); The method includes:

9. 9. The method according to claim 8, wherein the sample (6) is a contaminant present on a sampling surface of a sampling support made from a material transparent to gamma radiation, the method preferably further comprising a step of packaging the sample (6) in a compartment of the containment vessel (2), the packaging step comprising a step of assembling the sampling surface of the sampling support containing the contaminant by gluing it to a surface of a protective film (31), the protective film being made from a material transparent to alpha radiation, at least in an aperture (32) intended to face the contaminant.

10. 10. The method of claim 9, wherein the sampling support is made from polyethylene terephthalate (PET) and includes an adhesive layer on its sampling surface.

11. The sample (6) is a contaminant present on a sampling surface of a sampling support made of a material transparent to gamma radiation, the method preferably further comprising a step of packaging the sample (6) in a compartment of the containment vessel (2), the step of packaging comprising: - depositing said sample (6) on one face of a planar support (30) made of a material transparent to gamma radiation; - assembling by gluing the face of the planar support (30) on which the sample is deposited with the face of a protective film (31), said protective film being made of a material transparent to alpha radiation, at least in the apertures (32) intended to face the contaminant; 9. The method of claim 8, comprising:

12. 12. The method of claim 11, wherein the surface of the planar support (30) comprises an adhesive layer, the adhesive layer being present prior to the deposition of the sample (6).

13. The method according to claim 11 or claim 12, wherein the planar support (30) is made from polyethylene terephthalate (PET).

14. 14. The method according to any one of claims 9 to 13, wherein at least the apertures (32) of the protective film (31), preferably the entire protective film, are made from polyethylene terephthalate (PET).

15. The method of claim 14, wherein the aperture (32) in the PET protective film has a thickness of 6 μm or less.

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