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Development of neutron resonance transmission analysis as a non-destructive assay technique for nuclear nonproliferation

土屋 晴文; 北谷 文人; 前田 亮; 藤 暢輔; 呉田 昌俊

Plasma and Fusion Research (Internet), 13(Sp.1), p.2406004_1 - 2406004_4, 2018/02



Neutron resonance analysis for nuclear safeguards and security applications

Paradela, C.*; Heyse, J.*; Kopecky, S.*; Schillebeeckx, P.*; 原田 秀郎; 北谷 文人; 小泉 光生; 土屋 晴文

EPJ Web of Conferences (Internet), 146, p.09002_1 - 09002_4, 2017/09

Neutron-induced reactions can be used to study the properties of nuclear materials in the field of nuclear safeguards and security. The elemental and isotopic composition of these materials can be determined by using the presence of resonance structures in the reaction cross sections as fingerprints. This idea is the basis of two non-destructive analytical techniques which have been developed at the GELINA neutron time-of-flight facility of the JRC-IRMM: Neutron Resonance Capture Analysis (NRCA) and Neutron Resonance Transmission Analysis (NRTA). A full quantitative validation of the NRTA technique was obtained by determining the areal densities of enriched reference samples used for safeguards applications with an accuracy better than 1%. Moreover, a combination of NRTA and NRCA has been proposed for the characterisation of particle-like debris of melted fuel formed in severe nuclear accidents. In order to deal with the problems due to the diversity in shape and size of these samples and the presence of strong absorbing matrix materials, new capabilities have been implemented in the resonance shape analysis code REFIT. They have been validated by performing a blind test in which the elemental abundance of a combined sample composed of unknown quantities of materials such as cobalt, tungsten, rhodium or gold was determined with accuracies better than 2%.


Influence of the neutron transport tube on neutron resonance densitometry

北谷 文人; 土屋 晴文; 小泉 光生; 高峰 潤; 堀 順一*; 佐野 忠史*

EPJ Web of Conferences (Internet), 146, p.09032_1 - 09032_3, 2017/09

The use of a short flight path is effective in the neutron resonance analysis. On the other hand, such a short path would reduce a time resolution in Time-Of-Flight (TOF) measurements. In order to investigate the effect of neutron flight-path length, we carried out Neutron Resonance Transmission Analysis (NRTA) experiments with a short neutron flight path at the Kyoto University Research Reactor Institute - Linear Accelerator (KURRI-LINAC). In measurements of Neutron Resonance Densitometry, the quantity of nuclear materials is determined from TOF spectra obtained in the neutron energy range below 30 eV. Performing NRTA experiments with a 7-m flight path at KURRI-LINAC, we examined effects of flight path and pulse width on a TOF spectrum. A resonance dip of $$^{183}$$W at 27 eV in a TOF spectrum was successfully observed with an electron pulse width less than 2 $$mu$$s. In this presentation, we will discuss importance of the pulse width and short flight path to study design of a compact TOF facility to quantify nuclear materials.


Development of active neutron NDA techniques for nuclear nonproliferation and nuclear security

藤 暢輔; 大図 章; 土屋 晴文; 古高 和禎; 北谷 文人; 米田 政夫; 前田 亮; 呉田 昌俊; 小泉 光生; 瀬谷 道夫; et al.

EUR-28795-EN (Internet), p.684 - 693, 2017/00

In 2015, Japan Atomic Energy Agency (JAEA) and the Joint Research Centre (JRC) of the European Commission collaboration started to develop an active neutron non-destructive assay system for nuclear nonproliferation and nuclear security. To the best of our knowledge, no adequate technique exists that allows us to determine the amount of special nuclear materials and minor actinides in high radioactive nuclear materials, such as spent fuel, transuranic waste, etc. The collaboration aims at contributing to the establishment of an innovative NDA system using a D-T pulsed neutron source for various applications. We utilize several active neutron NDA techniques, namely Differential Die-Away Analysis (DDA), Prompt Gamma-ray Analysis (PGA), Neutron Resonance Capture Analysis (NRCA), Neutron Resonance Transmission Analysis (NRTA) and Delayed Gamma Spectroscopy (DGS). All of these techniques have advantages and disadvantages. The different methods can provide complementary information which is particularly useful for nuclear nonproliferation and nuclear security. In this project, we have developed a combined NDA system, which enables the measurements of DDA and PGA, at NUclear fuel Cycle safety Engineering research Facility (NUCEF) in JAEA. In this presentation, we will introduce our project and report the recent progress of developments, especially in NRTA, DDA and PGA.


LaBr$$_3$$ $$gamma$$-ray spectrometer for detecting $$^{10}$$B in debris of melted nuclear fuel

小泉 光生; 土屋 晴文; 北谷 文人; 原田 秀郎; Heyse, J.*; Kopecky, S.*; Mondelaers, W.*; Paradela, C.*; Schillebeeckx, P.*

Nuclear Instruments and Methods in Physics Research A, 837, p.153 - 160, 2016/11

Neutron Resonance Densitometry (NRD) has been proposed as a non-destructive analytical method for quantifying Special Nuclear Material (SNM) in the rock- and particle-like debris that is to be removed from the Fukushima Daiichi Nuclear Power Plant. The method is based on Neutron Resonance Transmission Analysis (NRTA) and Neutron Resonance Capture Analysis combined with Prompt Gamma Ray Analysis (NRCA/PGA). Although quantification of SNM will predominantly rely on NRTA, this will be hampered by the presence of strong neutron-absorbing matrix materials, in particular $$^{10}$$B. Results obtained with NRCA/PGA are used to improve the interpretation of NRTA data. Prompt $$gamma$$-rays originating from the $$^{10}$$B(n, $$alphagamma$$) reaction are used to assess the amount of $$^{10}$$B. The 478 keV $$gamma$$-rays from $$^{10}$$B, however, need to be measured under a high-radiation environment, especially from $$^{137}$$Cs. In order to meet this requirement, we have developed a well-shaped $$gamma$$-ray spectrometer consisting of a cylindrical and four rectangular cuboid LaBr$$_3$$ scintillators, and a fast data acquisition system.


Overview of JENDL-4.0/HE and benchmark calculations

国枝 賢; 岩本 修; 岩本 信之; 湊 太志; 岡本 力; 佐藤 達彦; 中島 宏; 岩元 洋介; 岩元 大樹; 北谷 文人; et al.

JAEA-Conf 2016-004, p.41 - 46, 2016/09



Development of active neutron NDA techniques for nonproliferation and nuclear security, 2; Study on a compact NRTA system

土屋 晴文; 北谷 文人; 前田 亮; 呉田 昌俊

Proceedings of INMM 57th Annual Meeting (Internet), 6 Pages, 2016/07

近年、核保障措置や核セキュリティの観点から、使用済み燃料や次世代のMA-Pu燃料、燃料デブリ中の核物質を非破壊により測定する重要性が増している。その重要性に叶う非破壊分析技術の一つに中性子共鳴透過分析法[Neutron Resonance Transmission Analysis(NRTA)]がある。NRTAは中性子飛行時間測定技術に立脚した技術で、精密さが要求される核データ測定に長年、使われている。実際、核物質の定量にNRTAが有効であることは、これまでの原子力機構とJRCとの共同実験により示されている。ゆえに、NRTAは現在の核不拡散・核セキュリティ分野の必要性にまさに叶うと考えている。しかしながら、今までのNRTA装置は大型の電子線加速器施設を利用しているため、汎用性に欠ける一面があった。そこで、われわれはD-T管(パルス幅10マイクロ秒、平均最大強度$$10^{8}$$から$$2times10^{9}$$ n/s)を利用した小型NRTA装置のプロトタイプの開発に着手した。本発表では、プロトタイプ装置の概要と、プロトタイプ装置の使用済み核燃料やMA-Pu燃料に対する適用性を数値計算により評価した結果を報告する。また、将来的には小型電子線加速器を用いたNRTA装置を開発することを視野に入れており、小型電子線加速器を用いたNRTA装置の性能についても議論する。



北谷 文人

核データニュース(インターネット), (114), p.44 - 49, 2016/06



Measurement of the $$^{77}$$Se($$gamma$$, n) cross section and uncertainty evaluation of the $$^{79}$$Se(n, $$gamma$$) cross section

北谷 文人; 原田 秀郎; 後神 進史*; 岩本 信之; 宇都宮 弘章*; 秋宗 秀俊*; 豊川 弘之*; 山田 家和勝*; 井頭 政之*

Journal of Nuclear Science and Technology, 53(4), p.475 - 485, 2016/04


We precisely measured the ($$gamma$$, n) cross section for $$^{77}$$Se by developing a spectroscopic method utilizing Laser Compton-Scattering $$gamma$$-rays. Moreover, the $$^{79}$$Se(n, $$gamma$$) $$^{80}$$Se cross section was deduced using the statistical model calculation code CCONE with $$gamma$$-ray strength functions adjusted to reproduce the ($$gamma$$, n) cross sections for $$^{77}$$Se and the even Se isotopes $$^{76}$$Se, $$^{78}$$Se and $$^{80}$$Se. The reliability of the $$^{79}$$Se(n, $$gamma$$) $$^{80}$$Se cross section calculated by CCONE with the adjusted $$gamma$$-ray strength function was evaluated by comparing available experimental (n, $$gamma$$) cross sections for stable $$^{76, 77}$$Se isotopes and those calculated by CCONE with the adjusted $$gamma$$-ray strength function. The result provides fundamental data for the study of nuclear transmutation for the long-lived fission product of $$^{79}$$Se.


Current activities and future plans for nuclear data measurements at J-PARC

木村 敦; 原田 秀郎; 中村 詔司; 岩本 修; 藤 暢輔; 小泉 光生; 北谷 文人; 古高 和禎; 井頭 政之*; 片渕 竜也*; et al.

European Physical Journal A, 51(12), p.180_1 - 180_8, 2015/12

In order to improve the data accuracy of neutron-capture cross sections of minor actinides (MAs) and long-lived fission products (LLFPs), a new experimental instrument named "Accurate Neutron-Nucleus Reaction measurement Instrument (ANNRI)" has been constructed in the Materials and Life science experimental Facility (MLF) at the Japan Proton Accelerator Research Complex (J-PARC), and measurements of neutron-capture cross sections of MAs, LLFPs and some stable isotopes with high intensity pulsed neutrons have been started. The analyses for $$^{244}$$Cm, $$^{246}$$Cm, $$^{241}$$Am and $$^{237}$$Np were finished; those for $$^{129}$$I, $$^{107}$$Pd, $$^{99}$$Tc, $$^{93}$$Zr and some stable isotopes are in progress. These results will make significant contributions in the field of developing innovative nuclear systems.


中性子共鳴濃度分析法の性能評価,2; 中性子共鳴捕獲$$gamma$$線分析法

土屋 晴文; 原田 秀郎; 小泉 光生; 北谷 文人; 呉田 昌俊; Becker, B.*; Kopecky, S.*; Heyse, J.*; Paradela, C.*; Mondelaers, W.*; et al.

核物質管理学会(INMM)日本支部第36回年次大会論文集(インターネット), 9 Pages, 2015/12

粒子状の溶融燃料デブリに含まれるウランやプルトニウム同位体を非破壊で定量することを目的に、中性子共鳴濃度分析法(NRD)の技術開発を進めてきた。NRDは、中性子共鳴透過分析法(NRTA)に中性子共鳴捕獲$$gamma$$線分析法(NRCA)、あるいは即発$$gamma$$線分析法(PGA)を組み合わせた技術である。NRDにおけるNRCA/PGAの役割は、主に$$^{137}$$Csによる高放射線場においてデブリ中の原子炉や建屋の構造材、ボロンなどの不純物を同定することである。これを実現するため、LaBr$$_3$$結晶を用いた新型の$$gamma$$線検出器やそれ専用の遮蔽体を開発した。これらの$$gamma$$線検出器や遮蔽体を用いて、ベルギーの中性子飛行時間施設GELINAにおいて公開デモ実験を実施した結果、第三者によってブラックボックス内に密封された試料(Hf, Gd, Ni)を同定することに成功した。本発表では、開発した$$gamma$$線検出器の設計概念と測定原理、及びNRCAデモ実験結果について報告する。


中性子共鳴濃度分析法の性能評価,1; 中性子共鳴透過分析法

北谷 文人; 原田 秀郎; 小泉 光生; 土屋 晴文; 呉田 昌俊; Becker, B.*; Kopecky, S.*; Heyse, J.*; Paradela, C.*; Mondelaers, W.*; et al.

核物質管理学会(INMM)日本支部第36回年次大会論文集(インターネット), 9 Pages, 2015/12

平成24年度から平成26年度にかけて、粒子状の溶融燃料デブリに含まれるウランやプルトニウム同位体を非破壊で定量する技術として、中性子共鳴濃度分析法(NRD)の開発を進めてきた。NRDは、中性子共鳴透過分析法(NRTA)と中性子共鳴捕獲$$gamma$$線分析法(NRCA)あるいは即発$$gamma$$線分析法(PGA)を組み合わせた技術である。NRDにおけるNRTAの役割は、溶融燃料デブリ中の核燃料物質(U, Pu等)の同位体を定量することである。この目的のために飛行時間法(Time of Flight: TOF)を利用した中性子吸収測定を実施する。これについて。ベルギーの中性子飛行時間施設GELINAにて性能評価デモ実験を実施した。その結果、Au, W, Rh, Nb, Cu. Co, Mn, Bをランダムに選択して、封をされたブラックボックス内の試料を定量することに成功した。本発表では、開発したNRTAの測定原理を述べ、実施したデモ実験の詳細を発表する。


Technique of neutron resonance transmission analysis for active neutron NDA

土屋 晴文; 小泉 光生; 北谷 文人; 呉田 昌俊; 原田 秀郎; 瀬谷 道夫; Heyse, J.*; Kopecky, S.*; Mondelaers, W.*; Paradela, C.*; et al.

Proceedings of 37th ESARDA Annual Meeting (Internet), p.846 - 851, 2015/08



Techniques of neutron resonance capture analysis and prompt $$gamma$$-ray analysis for active neutron NDA

小泉 光生; 土屋 晴文; 北谷 文人; 呉田 昌俊; 瀬谷 道夫; 原田 秀郎; Heyse, J.*; Kopecky, S.*; Mondelaers, W.*; Paradela, C.*; et al.

Proceedings of 37th ESARDA Annual Meeting (Internet), p.852 - 858, 2015/08

Active NDA techniques will draw out more information on the sample objects, in comparison with passive NDA techniques. Elementary particles (such as photons and neutrons) are used to induce nuclear reactions in the sample objects. The materials in the objects are deduced from the measured particles coming out of them. A new development program of active neutron NDA technologies has been started for detection/measurement of nuclear materials using a pulsed neutron source for nuclear security and nuclear non-proliferation; this project includes the basic technological development of NRTA, NRCA/PGA, neutron differential die-away (DDA) and a Delayed Gamma-ray (DG) technique. A system of active neutron NDA has been proposed. In this presentation, we review the methods and techniques on NRCA and PGA, which will be utilized for identifying materials in the objects in active neutron NDA.


Superdeformation in $$^{35}$$S

郷 慎太郎*; 井手口 栄治*; 横山 輪*; 小林 幹*; 木佐森 慶一*; 高木 基伸*; 宮 裕之*; 大田 晋輔*; 道正 新一郎*; 下浦 享*; et al.

JPS Conference Proceedings (Internet), 6, p.030005_1 - 030005_4, 2015/06

The high-spin states in $$^{35}$$S were investigated at Tandem-ALTO facility in Institut de Physique Nucl$'e$aire d'Orsay The $$^{26}$$Mg($$^{18}$$O, 2$$alpha$$1n)$$^{35}$$S fusion evaporation reaction was used to populate high-spin states in $$^{35}$$S. The germanium $$gamma$$-ray detector array ORGAM was employed to measure $$gamma$$ rays from high-spin states and charged particles evaporated from the compound nuclei were detected by a segmented silicon detector, Si-Ball. A level scheme for $$^{35}$$S was deduced based on the gamma-gamma-coincidence analysis and $$gamma$$-ray angular correlation analysis. The half-life of the transition in the superdeformed band was estimated by measuring the residual Doppler shift. The deduced half-life shows the large collectivity of the band.


Generalized analysis method for neutron resonance transmission analysis

原田 秀郎; 木村 敦; 北谷 文人; 小泉 光生; 土屋 晴文; Becker, B.*; Kopecky, S.*; Schillebeeckx, P.*

Journal of Nuclear Science and Technology, 52(6), p.837 - 843, 2015/06


Neutron resonance densitometry (NRD) is a non-destructive analysis method, which can be applied to quantify special nuclear materials (SNM) in small particle-like debris of melted fuel that is formed in severe accidents of nuclear reactors such as the Fukushima Daiichi Nuclear Power Plants. NRD uses neutron resonance transmission analysis (NRTA) to quantify SNM and neutron resonance capture analysis (NRCA) to identify matrix materials and impurities. In order to generalize NRD for the characterization of arbitrary-shaped thick materials, a generalized method to analyze NRTA data has been developed. The method has been applied on data resulting from transmission through non-uniform thick samples with varying areal density of SNM up to 0.253 at/b ($$approx$$100 g/cm$$^{2}$$). The investigation shows that NRD could be used to quantify SNM in not only uniform samples made of small particle-like debris but also non-uniform samples made of large rock-like debris with high accuracy by utilizing the generalized analysis method for NRTA.


NRD demonstration experiments at GELINA

Paradela, C.*; Alaerts, G.*; Becker, B.*; 原田 秀郎; Heyse, J.*; 北谷 文人; 小泉 光生; Kopecky, S.*; Mondelaers, W.*; Moens, A.*; et al.

EUR-27507-EN, 16 Pages, 2015/04

Neutron Resonance Densitometry (NRD), a non-destructive analysis method, is presented. The method has been developed to quantify special nuclear material (SNM) in debris of melted fuel that will be produced during the decommissioning of the Fukushima Daiichi Nuclear Power Plants. The method is based on Neutron Resonance Transmission Analysis (NRTA) and Neutron Resonance Capture Analysis (NRCA). The quantification of SNM relies on the NRTA results. The basic principles of NRD, which are based on well-established methodologies for neutron resonance spectroscopy, are explained. To develop NRD for the characterization of rock- and particle like heterogeneous samples a JAEA/JRC collaboration has been established. As part of this collaboration a NRD demonstration workshop was organized at the TOF facility GELINA of the JRC-IRMM. The results of this workshop are presented. They illustrate the potential of measurements of complex mixtures of different elements. It is demonstrated that the elemental composition of an unknown sample predicted by NRTA deviated on average by less than 2% from the declared value. In addition the potential to identify the presence of light elements by NRCA is shown.


Misassigned neutron resonances of $$^{142}$$Nd and stellar neutron capture cross sections

片渕 竜也*; 松橋 泰平*; 寺田 和司; 井頭 政之*; 水本 元治*; 廣瀬 健太郎; 木村 敦; 岩本 信之; 原 かおる*; 原田 秀郎; et al.

Physical Review C, 91(3), p.037603_1 - 037603_5, 2015/03


Time-of-flight spectra of the neutron capture events of $$^{142}$$Nd were measured using a spallation neutron source at the Japan Proton Accelerator Research Complex. The first six resonances of $$^{142}$$Nd reported in a previous work were not observed. The experimental results and cross-search of resonance energies in nuclear data libraries suggested that resonances of impurity nuclide $$^{141}$$Pr have been mistakenly assigned as $$^{142}$$Nd in the previous experiment. To investigate the impact of non-existence of the resonances to the s-process nucleosynthesis model, the Maxwellian averaged neutron capture cross sections with and without the misassigned resonances were compared.


Response function for the measurement of (n,$$gamma$$) reactions with the ANNRI-Cluster Ge detectors at J-PARC

原 かおる; 後神 進史*; 原田 秀郎; 廣瀬 健太郎; 木村 敦; 金 政浩*; 北谷 文人; 小泉 光生; 中村 詔司; 藤 暢輔; et al.

JAEA-Conf 2014-002, p.88 - 92, 2015/02

Recently, neutron shields of a large Ge detector array at the Accurate Neutron-Nucleus Reaction Measurement Instrument (ANNRI) in the Japan Proton Accelerator Research Complex (J-PARC) were modified to suppress the background from boron rubber sheets to enriched $$^{6}$$LiF tiles. For the new experimental set-up, efficiencies and response functions of the cluster Ge detectors with the BGO anti-coincidence detectors were measured with $$gamma$$-rays from standard sources and prompt $$gamma$$-rays from the $$^{28}$$Si(n,$$gamma$$) and $$^{35}$$Cl(n,$$gamma$$) reactions. The simulation parameters were adjusted with the EGS5 code so as to reproduce the data set of efficiencies and response functions. Based on this information, a pulse height weighting function will be deduced in the energy range of 0.1-10 MeV.


NRDの開発,3; 小型14MeVパルス中性子源に用いる新型モデレータの研究

高峰 潤; 小泉 光生; 呉田 昌俊; 原田 秀郎; 北谷 文人; 土屋 晴文; 瀬谷 道夫; 飯村 秀紀

核物質管理学会(INMM)日本支部第35回年次大会論文集(インターネット), 10 Pages, 2015/01


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