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Towards Developing Minor Actinides Transmutation Systems
−Improving the Accuracy of the Experimental Nuclear Data for 241Am at J-PARC−


Fig.1 Comparison with the past experimental data and JENDL-5

Fig. 1 Comparison with the past experimental data and JENDL-5

Accuracy improvement achieved in terms of resonance area (a), cross-section value and reduction of uncertainty (b).

 Highly accurate nuclear data are required for the development of nuclear transmutation systems, which are meant to convert minor actinides (MAs), such as 241Am, into short-lived or stable nuclei. Nuclear data for a multitude of reactions and isotopes, which are essential for the system design, are compiled in different nuclear data libraries, such as JENDL-5, which is developed by JAEA. However, to implement transmutation systems, the present nuclear data for MAs needs to be improved. In particular, further experimental results are required for the 241Am neutron capture cross-section to resolve the discrepancies over 15 % in low-energy resonances between different nuclear data libraries, as well as an accuracy increase above 1000 eV of the cross-section with an uncertainty reduction as close to 5 % as possible, since even a few percentage reductions in the experimental uncertainty can significantly increase the nuclear data accuracy and highly impact the reactor design.
 In this study, an experimental technique was developed to measure the neutron capture cross-section of 241Am with high accuracy at the ANNRI beamline of J-PARC, which is the most powerful neutron beam in the world, based on: (1) data cuts to remove the background events, (2) background estimations using resonances, (3) a normalization independent from nuclear data and (4) correction for missed γ-rays. This technique enables the acquisition of highly accurate results using small amounts of 241Am, reducing sample radioactivity and minimizing its systematic effects.
 The present results revealed an overestimation in the low-energy resonance areas by about 10 %, well as a large underestimation of the cross-section between 1000 and 10000 eV by 30–70 % in JENDL-5 while providing much lower uncertainties compared to past data (15–45 % to 10–20 %), as can be seen in Fig. 1a and Fig.1b, respectively.
 This increase in experimental accuracy achieved will contribute to improving the accuracy of the nuclear data in libraries for 241Am, thereby advancing the development of transmutation systems.

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  • (1)Data cuts to remove background events

     In the experiments, the neutron capture cross-section is derived from measuring the γ-rays emitted in such reaction. Nonetheless, γ-rays emitted from other reactions and sources can also be recorded inducing intro background noise. To improve the signal-to-noise ratio, data cuts were applied to the detected γ-rays based on its energy. When a neutron capture reaction occurs, γ-rays are emitted with energies relative to the excited state of the measured isotope. In the case of 241Am, γ-rays are emitted after a capture event have energies up to about 5.6 MeV. Hence, a data cut at 5.6 MeV was applied to the measured events, since γ-rays over such energy necessarily come from a background source. This is particularly important in the present experimental setup, since neutron captured in the I present in the NaI(Tl) detector are a large source of γ-ray noise with energies between 6.5 and 7 MeV. Moreover, events with energies of 478 and 511 keV are another large source of background events. The former originates from neutrons capture in boron, extensively used as neutron shielding, whereas 511 keV is the energy equivalent of an electron, which are generated by the interaction of γ-rays with surrounding materials. Hence, to reduce the influence of background events and improve the experimental accuracy, data cuts were performed at 0.6 and 6 MeV, removing the influence of high and lower energy γ-rays. These peaks, as well as the data cuts applied, can be seen clearly in the raw γ-ray spectra of the different measured samples shown in Fig. 2.

  • Fig.2   Measured γ-ray from the different samples together with the data cuts applied

    Fig. 2 Measured γ-ray from the different samples together with the data cuts applied

  • (2) Background estimation using resonances

     When measurements are performed, a large amount of background γ-rays are detected together with capture γ-rays coming from the measured sample. This background level becomes quite significant when the sample employed has a very small mass, and also is sealed in case, which was the case for the 241Am, since it is highly radioactive. This is background is estimated and then removed through the measurement of other samples and a non-sample measurement. The most important background for 241Am, was that caused by the sample case along with a small amount of Yttrium that was used as binder. The typical approach would be to rely in the Yttrium mass amounts provided by the supplier. However, these values carry a substantial amount of uncertainty since they are hard to quantify. Hence, in the present analysis, for a more accurate assessment of the background events caused by the sample case, the background normalization relied in physical phenomena, in this case the resonances caused by neutrons interacting with Yttrium, that display an extremely high degree of correlation to the amount of Yttrium irradiated, and also accounts for any flux attenuation within the sample. The measured spectra for both the 241Am and dummy case samples is displayed in Fig. 3, with the Yttrium resonance used to normalize the background shown in the in-plot.

  • Fig. 3  Dummy spectra normalized using the resonance of Yttrium

    Fig. 3 Dummy spectra normalized using the resonance of Yttrium

  • (3) Normalization independent from nuclear data

     The cross-section is determined as the number of capture events induced in the sample per number incident neutron, and accounting for the area density of the sample. However, the final results have to be normalized since the capture events and the incident neutrons are determined from different measurements with distinct detection efficiencies. The most common approach involves the use of a well-known cross-section value present in evaluated nuclear data libraries, such as JENDL-5. Nonetheless, this procedure introduces the uncertainty present in nuclear data libraries, which is non-negligible. To avoid that, the present results were normalized using the saturated resonance technique, which is based on measuring an element that has a large capture resonance with a thick enough sample for that resonance to be completely saturated. This means that all neutrons with the energy of that resonance interact with the sample and, hence, the event rate attained at that resonance is equal to the incident neutron flux, accounting for 2 % of the neutrons being backscattered. The saturation achieved with a 0.1 mm thick 197Au sample is shown in Fig. 4, as well as the normalized neutron flux to that resonance. Thus, by relying on a physical constrain, the final cross-section results were attained independent from other nuclear data.

  • Fig. 4  Normalized neutron flux to the saturated resonance of 197Au

    Fig. 4 Normalized neutron flux to the saturated resonance of 197Au

  • (4) Correction for missed γ-rays

     To reduce the influence of the background events, events with energies below 0.6 MeV were not considered in the analysis, as shown above. This means that capture γ-rays with energies below 0.6 MeV were also missed, but this fact does not introduce any energy-dependent bias in the cross-section results. However, since the results were normalized using the capture data of 197Au with the saturated resonance technique, the ratio of the missed γ-ray below 0.6 MeV relative to the total γ-rays emitted ratio is different between 241Am and 197Au and needs to be taken into account. 197Au emits capture γ-rays up to 6.5 MeV, much higher than the 5.6 MeV limit for 241Am. This difference was corrected using the γ-rays spectra calculated using the nuclear reaction model code CCONE for both 241Am and 197Au. The calculated γ-ray spectra from CCONE for both isotopes are shown in comparison with that derived from the experimental work in Fig. 5.

  • Fig. 5  Experimental and calculated capture γ-ray spectra from 241Am and 197Au

    Fig. 5 Experimental and calculated capture γ-ray spectra from 241Am and 197Au


  • Author (Researcher) Information

    Name | Gerard Rovira
    Nuclear Data Center, Nuclear Science and Engineering Center, Nuclear Science Research Institute

    Reference

    Rovira, G. et al., 241AM Neutron Capture Cross Section Measurement Using the Nai(TL) Spectrometer of the Annri Beamline of J-Parc, Journal of Nuclear Science and Technology, vol.61, issue 4, 2024, p.459–477.

    Paper URL: https://doi.org/10.1080/00223131.2023.2239885

    January 7, 2025

     Nuclear Science and Engineering Research 

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