和田 有希*; 中澤 知洋*; 榎戸 輝揚*; 古田 禄大; 湯浅 孝行*; 牧島 一夫*; 土屋 晴文
Physical Review D, 101(10), p.102007_1 - 102007_6, 2020/05
During a winter thunderstorm on November 24, 2017, a downward terrestrial gamma-ray flash took place and triggered photonuclear reactions with atmospheric nitrogen and oxygen nuclei, coincident with a lightning discharge at the Kashiwazaki-Kariwa nuclear power station in Japan. We directly detected neutrons produced by the photonuclear reactions with gadolinium orthosilicate scintillation crystals installed at sea level. Two gadolinium isotopes included in the scintillation crystals, Gd and Gd, have large cross sections of neutron captures to thermal neutrons such as Gd(n,)Gd and Gd(n,)Gd. De-excitation gamma rays from Gd and Gd are self-absorbed in the scintillation crystals, and make spectral-line features which can be distinguished from other non-neutron signals. The neutron burst lasted for 100 ms, and neutron fluences are estimated to be 58 and 31 neutrons cm at two observation points at the power plant. Gadolinium orthosilicate scintillators work as valid detectors for thermal neutrons in lightning.
Ma, F.; Kopecky, S.*; Alaerts, G.*; 原田 秀郎; Heyse, J.*; 北谷 文人; Noguere, G.*; Paradela, C.*; alamon, L.*; Schillebeeckx, P.*; et al.
Journal of Analytical Atomic Spectrometry, 35(3), p.478 - 488, 2020/03
The use of Neutron Resonance Transmission Analysis to characterize homogeneous samples not fulfilling good transmission geometry conditions is discussed. Analytical expressions for such samples have been derived and implemented in the resonance shape analysis code REFIT. They were validated by experiments at the time-of-flight facility GELINA using a set of metallic natural copper samples. The expressions were used to derive sample characteristics by a least squares adjustment to experimental transmission data. In addition, the resonance parameters of Cu for energies below 6 keV, which are reported in the literature and recommended in evaluated data libraries, were verified. This research was implemented under the subsidiary for nuclear security promotion of MEXT.
和田 有希*; 榎戸 輝揚*; 中澤 知洋*; 古田 禄大; 湯浅 孝行*; 中村 佳敬*; 森本 健志*; 松元 崇弘*; 牧島 一夫*; 土屋 晴文
Physical Review Letters, 123(6), p.061103_1 - 061103_6, 2019/08
During a winter thunderstorm on 2017 November 24, a strong burst of gamma-rays with energies up to 10 MeV was detected coincident with a lightning discharge, by scintillation detectors installed at Kashiwazaki-Kariwa Nuclear Power Plant at sea level in Japan. The burst had a sub-second duration, which is suggestive of photoneutron productions. The leading part of the burst was resolved into four intense gamma-ray bunches, each coincident with a low-frequency radio pulse. These bunches were separated by 0.71.5 ms, with a duration of 1 ms each. Thus, the present burst may be considered as a "downward" terrestrial gamma-ray flash (TGF), which is analogous to up-going TGFs observed from space. Although the scintillation detectors were heavily saturated by these bunches, the total dose associated with them was successfully measured by ionization chambers, employed by nine monitoring posts surrounding the power plant. From this information and Monte Carlo simulations, the present downward TGF is suggested to have taken place at an altitude of 2500500 m, involving avalanche electrons with energies above 1 MeV which is comparable to those in up-going TGFs.
土屋 晴文; 小泉 光生; 北谷 文人; 原田 秀郎
Nuclear Instruments and Methods in Physics Research A, 932, p.16 - 26, 2019/07
A large-volume (12.0 cm12.7 cm) LaBr scintillation detector equipped with a specially-designed radiation shield was evaluated for neutron resonance capture analysis at the neutron time-of-flight (TOF) facility GELINA. By using the LaBr detector with and without the shield, measurements were carried out at a 13-m TOF station with three metallic samples, namely, Ni, Cr, and Fe. In addition, Monte Carlo simulations with Geant4 were performed, and the results were compared with the measurements to analyze the observed energy spectra and TOF spectra. Energy spectra obtained with the shield showed that prompt -ray peaks emitted from each sample can be used to identify the isotopes. Moreover, the signal-to-noise ratios of resonance peaks in a TOF spectrum with the shield were enhanced 1.5-2.5 in comparison with those without the shield. Furthermore, simultaneous measurements conducted using the three samples demonstrated that the shield employed herein was indispensable for identifying impurities in a composite sample such as particle-like fuel debris.
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; 小泉 光生
Proceedings of INMM 60th Annual Meeting (Internet), 7 Pages, 2019/07
Nuclear material accountancy plays a key role in nuclear safeguards and security. The collaboration between the Japan Atomic Energy Agency (JAEA) and the Joint Research Centre (JRC) of the European Commission aims to develop an active neutron NDA system for Special Nuclear Materials (SNM) and Minor Actinides (MA) in highly radioactive nuclear materials. 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-ray Analysis (DGA) have been developed. The different methods can provide complementary information. In the first phase of the project, we developed a combined NDA system, which enables the simultaneous measurements of DDA and PGA. The DDA technique can determine very small amounts of the fissile mass. PGA is valuable for the measurement of light elements. In the second phase, we will continue to conduct additional research to improve the methodology and develop a new integrated NDA system which can use for NRTA as well as DDA and PGA. In this presentation, we will provide an overview of the project and report the recent results, especially the design of new integrated NDA system. This research was implemented under the subsidiary for nuclear security promotion of MEXT.
和田 有希*; 榎戸 輝揚*; 中村 佳敬*; 古田 禄大; 湯浅 孝行*; 中澤 知洋*; 森本 健志*; 佐藤 光輝*; 松元 崇弘*; 米徳 大輔*; et al.
Communications Physics (Internet), 2(1), p.67_1 - 67_9, 2019/06
Two types of high-energy events have been detected from thunderstorms. One is "terrestrial gamma-ray flashes" (TGFs), sub-millisecond emissions coinciding with lightning discharges. The other is minute-lasting "gamma-ray glows". Although both phenomena are thought to originate from relativistic runaway electron avalanches in strong electric fields, the connection between them is not well understood. Here we report unequivocal simultaneous detection of a gamma-ray glow termination and a downward TGF, observed from the ground. During a winter thunderstorm in Japan on 9 January 2018, our detectors caught a gamma-ray glow, which moved for 100 s with ambient wind, and then abruptly ceased with a lightning discharge. Simultaneously, the detectors observed photonuclear reactions triggered by a downward TGF, whose radio pulse was located within 1 km from where the glow ceased. It is suggested that the highly-electrified region producing the glow was related to the initiation of the downward TGF.
土屋 晴文; Ma, F.; 北谷 文人; Paradella, C.*; Heyse, J.*; Kopecky, S.*; Schillebeeckx, P.*
Proceedings of 41st ESARDA Annual Meeting (Internet), p.374 - 377, 2019/05
From a viewpoint of nuclear safeguards and nuclear security, non-destructive assay (NDA) techniques are needed to quantify special nuclear materials (SNMs) in nuclear fuels such as spent fuels and fuel debris. Neutron Resonance Transmission Analysis (NRTA) is an NDA technique and it measures the amount of U isotopes in a UO sample within 1% accuracy and Pu isotopes in a PuO sample within 5% accuracy. However, NRTA measurements done so far were mainly applied to homogeneous samples with a constant thickness. Spent fuel and especially debris have irregular shapes that affect the NRTA measurements. In order to investigate the influence of irregular-shaped samples, NRTA experiments were done with a copper bar sample with different rotation angles with respect to neutron beams, at a neutron Time-Of-Flight (TOF) facility GELINA (Belgium). Analytical models for irregular shaped samples proposed by Harada et al. (JNST, 2015) were applied to the experimental data. It has been found that the experimental data can be well reproduced by the proposed models. In this presentation, we report how analytical models are applied to a real NRTA experiment with a Cu bar sample and discuss a future prospect of a compact NRTA system for SNM quantification. This research was implemented under the subsidiary for nuclear security promotion of MEXT.
榎戸 輝揚*; 和田 有希*; 土屋 晴文
日本物理学会誌, 74(4), p.192 - 200, 2019/04
北谷 文人; 土屋 晴文; 藤 暢輔; 堀 順一*; 佐野 忠史*; 高橋 佳之*; 中島 健*
KURRI Progress Report 2017, P. 99, 2018/08
As a non-destructive analytical technique for nuclear material in the field of nuclear security and nuclear nonproliferation, a neutron resonance transmission analysis (NRTA) attracts attention of researchers. It is important to downsize a NRTA system when it is deployed at various facilities. For this aim, we have developed a compact NRTA system which utilizes a D-T neutron generator. Its pulse width of 10s is much longer than that of a large electron beam accelerator. It is necessary to understand the influence of pulse widths on the NRTA measurement. Therefore, we conducted the experiments of the simulated nuclear fuel pin samples to evaluate how the NRTA measurement is influenced by the pulse width of neutron beam. Experiments were performed in Kyoto University. The simulated fuel pellet sample was made from metallic powders of Ag (around 1%) and Al (around 99%). The energy of the irradiation neutron is determined by a Time of Flight technique. We used three pulse widths of the neutron beam of 0.1, 1 and 4 s. A resonance dip of Ag at 5.19 eV is observed in the all spectra. And the dip of the TOF spectrum shifts towards low energy, with pulse width changed to a longer one. In this work, we confirmed that neutron pulse width affected the NRTA measurement of the fuel pin sample. On the basis of this work, we will be able to quantify the effects of long-pulse width in a resonance analysis.
土屋 晴文; 北谷 文人; 藤 暢輔; Paradela, C.*; Heyse, J.*; Kopecky, S.*; Schillebeeckx, P.*
Proceedings of INMM 59th Annual Meeting (Internet), 6 Pages, 2018/07
In fields of nuclear safeguards and nuclear security, non-destructive assay (NDA) techniques are needed in order to quantify special nuclear materials (SNMs) in nuclear fuels. Among those techniques, active NDA ones would be preferable to passive ones. One candidate of active NDA techniques is neutron resonance transmission analysis (NRTA). In fact, experiments done at GELINA have shown that NRTA has high potential enough to quantify SNMs in complex materials. Currently, such a NRTA system requires a large electron accelerator facility to generate intense neutron sources. In other words, it is very difficult to perform NRTA at various facilities that need to measure SNMs. Thus, downsizing a NRTA system would be one solution of its difficulty. In order to realize a compact NRTA system, we develop a prototype with a D-T neutron generator that has a pulse width of 10 s. For this aim, numerical calculations to optimize the compact NRTA system were done. In addition, NRTA measurements with simulated fuel pins were made at neutron time-of-flight facilities such as GELINA. In this presentation, we present results of the numerical calculations and the experimental results. On the basis of those results we discuss a future prospect of a compact NRTA system that would be applicable to SNM quantification. This research was implemented under the subsidiary for nuclear security promotion of MEXT.
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; 小泉 光生; Heyse, J.*; Paradela, C.*; et al.
Proceedings of INMM 59th Annual Meeting (Internet), 9 Pages, 2018/07
Nuclear material accountancy is of fundamental importance for nuclear safeguards and security. However, to the best of our knowledge, there is no established technique that enables us to accurately determine the amount of Special Nuclear Materials (SNM) and Minor Actinides (MA) in high radioactive nuclear materials. Japan Atomic Energy Agency (JAEA) and the Joint Research Centre (JRC) of the European Commission Collaboration Action Sheet-7 started in 2015. The purpose of this project is to develop an innovative non-destructive analysis (NDA) system using a D-T pulsed neutron source. 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-ray Analysis (DGA) have been studied and developed. The different methods can provide complementary information which is particularly useful for quantification of SNM and MA in high radioactive nuclear materials. The second phase of the project has started. In the second phase, we will continue to conduct additional research to improve the methodology and develop an integrated NDA system. This presentation gives an overview of the project and the NDA system and reports the recent results. This research was implemented under the subsidiary for nuclear security promotion of MEXT.
和田 有希*; Bowers, G. S.*; 榎戸 輝揚*; 鴨川 仁*; 中村 佳敬*; 森本 健志*; Smith, D.*; 古田 禄大*; 中澤 知洋*; 湯浅 孝行*; et al.
Geophysical Research Letters, 45(11), p.5700 - 5707, 2018/06
An on-ground observation program for high energy atmospheric phenomena in winter thunderstorms along Japan Sea has been performed via lightning measurements of -ray radiation, atmospheric electric field and low-frequency radio band. On February 11, 2017, the radiation detectors recorded -ray emission lasting for 75 sec. The -ray spectrum extended up to 20 MeV and was reproduced by a cutoff power-law model with a photon index of 1.36, being consistent with a Bremsstrahlung radiation from a thundercloud (as known as a -ray glow). Then the -ray glow was abruptly terminated with a nearby lightning discharge. The low-frequency radio monitors, installed 50 km away from Noto School, recorded intra/inter-cloud discharges spreading over 60km area with a 300 ms duration. The timing of the -ray termination coincided with the moment when a sequence of intra/inter-cloud discharges passed 0.7 km horizontally away from the radiation monitors. The atmospheric electric-field measurement presented that negative charge was located in the cloud base and not neutralized by the lightning discharge. This indicates that the -ray source was located at an higher region than the cloud base.
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
榎戸 輝揚*; 和田 有希*; 古田 禄大*; 中澤 知洋*; 湯浅 孝行*; 奥田 和史*; 牧島 一夫*; 佐藤 光輝*; 佐藤 陽祐*; 中野 俊男*; et al.
Nature, 551(7681), p.481 - 484, 2017/11
Relativistic electrons accelerated by electric fields of lightnings and thunderclouds emit bremsstrahlung rays, which have been detected at ground observations. The energy of the rays is sufficiently high to potentially invoke atmospheric photonuclear reactions N(, n)N, which would produce neutrons and eventually positrons via decay of generated unstable radioactive isotopes, especially N. However, no clear observational evidence for the reaction has been reported to date. Here we report the first detection of neutron and positron signals from lightning with a ground observation. During a thunderstorm on 6 February 2017 in Japan, an intense -ray flash (1 ms) was detected at our monitoring sites. The subsequent initial burst quickly subsided with an exponential decay constant of 40-60 ms, followed by a prolonged line emission at 0.511MeV, lasting for a minute. The observed decay timescale and spectral cutoff at 10 MeV of the initial emission are well explained with de-excitation rays from the nuclei excited by neutron capture. The centre energy of the prolonged line emission corresponds to the electron-positron annihilation, and hence is the conclusive indication of positrons produced after the lightning. Our detection of neutrons and positrons is unequivocal evidence that natural lightning triggers photonuclear reactions.
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%.
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 W at 27 eV in a TOF spectrum was successfully observed with an electron pulse width less than 2 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.
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.
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 B. Results obtained with NRCA/PGA are used to improve the interpretation of NRTA data. Prompt -rays originating from the B(n, ) reaction are used to assess the amount of B. The 478 keV -rays from B, however, need to be measured under a high-radiation environment, especially from Cs. In order to meet this requirement, we have developed a well-shaped -ray spectrometer consisting of a cylindrical and four rectangular cuboid LaBr scintillators, and a fast data acquisition 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、平均最大強度から 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。
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)に中性子共鳴捕獲線分析法(NRCA)、あるいは即発線分析法(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結晶を用いた新型の線検出器やそれ専用の遮蔽体を開発した。これらの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。