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論文

Measurement of uranium and fission products in a spent fuel sample using fiber-optic laser-induced breakdown spectroscopy

Batsaikhan, M.; 大場 弘則*; 狩野 貴宏; 赤岡 克昭; 若井田 育夫*; 岩田 圭弘; 坂本 寛*

Journal of Analytical Atomic Spectrometry, 21 Pages, 2026/00

 被引用回数:0

This study presents the development and application of a fiber optic laser-induced breakdown spectroscopy system designed for remote, in situ analysis of nuclear fuel debris at Fukushima Daiichi Nuclear Power Station (FDNPS). The system was deployed for the first time in a hot cell under high radiation to analyse an actual Boiling Water Reactors spent fuel sample as an exemplar of FDNPS fuel debris. The system successfully identified the main fuel components along with several long lived fission products and related markers such as Sr, Cs, Mo, Ba, and Rb. The emission intensity of the Ba, Rb, and Cs near the periphery region was slightly higher than at the center of the fuel. This indicates a higher concentration of these elements in that area.

論文

$$>$$100 m fiber-coupled microchip laser-induced breakdown spectroscopy for remote elemental analysis applications

Batsaikhan, M.; 大場 弘則; 若井田 育夫

Optics Express (Internet), 32(25), p.45158 - 45170, 2024/12

 被引用回数:2 パーセンタイル:18.06(Optics)

This study aims to develop ultralong fiber optic cable (FOC) coupled microchip laser-induced breakdown spectroscopy (mLIBS) to reveal the elemental distribution and local composition of nuclear fuel debris in an accident-damaged reactors at Fukushima Daiichi Nuclear Power Station (FDNPS). Currently at FDNPS, the distance between the area where humans can safely work in a sufficient space and the nuclear fuel debris is expected to be over 100 m. Therefore, it becomes crucial to analyze the light transmittance performance of FOC-coupled mLIBS systems over such long distances in a high-radiation environment. We found that compared with an FOC with low-OH groups, that with high-OH groups exhibits better light transmittance performance. The maximum FOC length for microchip crystal oscillation is estimated to be longer than 800 m, although attenuation is observed with the increase in FOC length. Quantitative analysis of Gd is successfully performed in the visible region using the mLIBS system coupled with up to 300 m-long FOCs, with the limits of detection being between 0.1% and 0.2%.

論文

Effect of sample temperature and laser ablation angle on optical emission and acoustic signals from laser-induced Zirconium plasma

Batsaikhan, M.; 大場 弘則; 狩野 貴宏; 赤岡 克昭; 若井田 育夫

Optics Express (Internet), 32(24), p.42624 - 42638, 2024/11

 被引用回数:0 パーセンタイル:0.00(Optics)

A fiber-coupled, acoustic-wave-assisted microchip laser-induced breakdown spectroscopy system (AW-mLIBS) was developed to analyze the elemental composition and surface imaging. In this study, we measured the dependence of sample temperature and laser ablation angle on the laser-induced plasma-optical emission and LIP-acoustic signal. The intensity of the laser-induced plasma-optical emission and ablated mass at three different temperatures and eight different laser ablation angles were estimated using a zirconium sample. Simultaneously, we investigated the laser-induced plasma-acoustic signal amplitude, propagation speed, and shape by synchronizing the AW-mLIBS system with a high-speed camera. The results revealed that the laser-induced plasma-optical emission increases with increasing temperature and is unaffected by laser ablation angle up to 40 degree because the amount of the ablated mass was similar and the plasma. Additionally, no considerable variation in plasma temperature obtained using the Boltzmann method over the sample temperature. However, the propagation speed of the laser-induced plasma-acoustic signal differs with temperature but has marginal angular dependence because the laser-induced plasma-acoustic signal propagates as semispherical. Furthermore, small and no considerable changes observed in the laser-induced plasma-acoustic signal amplitude up to 100 degree Celsius, and the laser ablation angle showed a similar tendency to that of the laser-induced plasma-optical emission.

論文

Two-dimensional elemental mapping of simulated fuel debris using laser-induced breakdown spectroscopy

Batsaikhan, M.; 赤岡 克昭; 佐伯 盛久*; 狩野 貴宏; 大場 弘則; 若井田 育夫

Journal of Nuclear Science and Technology, 61(5), p.658 - 670, 2024/05

 被引用回数:2 パーセンタイル:30.64(Nuclear Science & Technology)

この実験研究では、レーザー誘起ブレークダウン分光法(LIBS)を用いて模擬燃料デブリの二次元元素マッピングを実行し、サンプル表面の元素組成と分布を決定した。本物の燃料デブリはサンプルとして入手できないため、化合物や金属などの予測材料から模擬燃料デブリを作製した。Nd:YAGレーザーの第2高調波を使用して、サンプル表面にプラズマを生成させた。さらに、エシェル分光器を使用して、435$$sim$$650nmの可視波長範囲でプラズマからの発光を検出した。収集されたデータセットのサイズと複雑さから従来のデータ分析方法では良い効果が得られないことが判明した。そのため本研究では、主成分分析や多変量曲線分解能代替最小二乗法などのラベルフリー化学測定法に基づく方法を実装して、サンプル内の各成分に関する空間情報およびスペクトル情報を取得した。結果として、LIBSと化学測定法の統合が、事前知識がほとんどまたは全く無くてもサンプル(燃料デブリなど)に関する定性情報を取得するための非常に効果的なツールであることを実証した。

論文

Simultaneous analysis of gadolinium and surface imaging using a fiber-coupled acoustic wave-assisted microchip LIBS system

Batsaikhan, M.; 大場 弘則; 狩野 貴宏; 赤岡 克昭; 若井田 育夫

Journal of Analytical Atomic Spectrometry, 39(2), p.423 - 432, 2024/02

 被引用回数:5 パーセンタイル:46.23(Chemistry, Analytical)

This paper reports a pioneering attempt at simultaneously analyzing gadolinium distribution and surface imaging of surrogate debris samples with homogeneous and heterogeneous composition using a fiber-coupled acoustic wave-assisted microchip laser-induced breakdown spectroscopy system. In this system, a microchip LIBS was used to measure the Gd distribution maps in the mixed oxide samples. Whereas, during elemental mapping by microchip LIBS, the laser-plasma acoustic waves were simultaneously recorded by microphone and applied for surface imaging of the samples. Additionally, the laser-plasma acoustic waves can be used to adjust the best-focusing position of the microchip LIBS because the acoustic wave amplitude is the strongest at the near best-focusing position. According to the measurement results, the emission spectra of the surrogate debris showed that the optical emission lines at 501.5 nm and 510.3 nm were suitable for Gd detection in the fuel debris sample. For Gd quantification, calibration curves were established from the intensity ratio of Gd and Ce emission lines. The surface imaging for the surrogate debris samples was successfully performed by collecting the laser-plasma acoustic waveforms during LIBS elemental mapping.

特許

レーザ装置、元素分析システム、及び元素分析方法

Batsaikhan, M.; 大場 弘則

not registered

特願 2023-119201  公開特許公報

【課題】レーザ光を用いて対象物に含有する元素を分析する際に、対象物の表面の破壊を抑制し、高精度な元素分析を可能とする。 【解決手段】対象物(M)に対してレーザ光(22)を照射するレーザ照射部(40)を備えたレーザ装置(30)において、レーザ光(22)の照射により対象物(M)から生じる音波(24)を取得する音波取得部(50)を備え、レーザ照射部(40)は、音波取得部(50)にて取得された音波に基づいて所定の焦点位置に制御される、ことを特徴とする。

口頭

Challenges for screening of nuclear fuel debris by innovative spectral imaging and its verification by LIBS mapping, 3; Detection of uranium in simulated fuel debris samples by acoustic wave-assisted microchip laser-induced breakdown spectroscopy

Batsaikhan, M.; 大場 弘則*; 狩野 貴宏; 岩田 圭弘; 赤岡 克昭; 若井田 育夫*; 坂口 知聡*; 坂本 寛*; 牟田 浩明*

no journal, , 

Remote, real time, accurate elemental analysis is essential at every stage of the safe and successful decommissioning of the Fukushima Daiichi Nuclear Power Station, from initial site characterization to storage of materials. This study presents the development of a novel acoustic wave assisted microchip laser induced breakdown spectroscopy technique for remote and real time elemental analysis and explores the use of laser induced plasma acoustic signal to optimize the lens to sample distance which is significantly affect to the signal intensity and accuracy of measurement. The analytical performance of the developed system was tested for uranium in mixed oxide samples and the limit of detection was evaluated to be 0.7 wt.% with calibration curve method.

口頭

Challenge for screening of nuclear fuel debris by innovative spectral imaging and its verification by LIBS mapping, 8; Elemental mapping of a heterogeneous UO$$_{2}$$-Zr-Fe sample using acoustic wave-assisted microchip LIBS

Batsaikhan, M.; 岩田 圭弘; 狩野 貴宏; 赤岡 克昭; 坂口 知聡*; 坂本 寛*; 牟田 浩明*

no journal, , 

We propose combining Hyperspectral Imaging (HSI) and Acoustic Wave-assisted microchip Laser-Induced Breakdown Spectroscopy (AW-mLIBS) techniques to identify in-core materials at the Fukushima Daiichi Nuclear Power Station (1F) in this project. This presentation will discuss the spatial analysis of U, Zr, and Fe in a heterogeneous UO$$_{2}$$-Zr-Fe sample.

口頭

マイクロ波重畳LIBSにおける焦点位置からの偏差の影響

狩野 貴宏; Batsaikhan, M.; 岩田 圭弘; 赤岡 克昭

no journal, , 

福島第一原子力発電所の廃止措置において、作業の効率化や安全性の確保する目的からレーザー誘起ブレークダウン発光分析法(LIBS)により燃料デブリ等を簡易分析することを提案している。LIBSではマイクロ波を用いることで発光強度を増強しS/N比を向上させることができるが、レーザーの焦点位置からズレた際にどのような影響があるか調べた。

口頭

Challenges for LIBS analysis of nuclear fuel debris at FDNPS; Effect of sample temperature and laser ablation angle on optical emission and acoustic signals from laser-induced Zirconium plasma

Batsaikhan, M.

no journal, , 

A fiber-coupled, acoustic wave assisted (AW) microchip laser induced breakdown spectroscopy (mLIBS) system is a promising tool for remote and on-site analysis of nuclear fuel debris formed in damaged reactor vessels at Fukushima Daiichi Nuclear Power Station. In the AW-mLIBS system, the laser induced plasma optical emission is used to measure the sample's elemental composition. The acoustic signal is recorded as an auxiliary source of information for optimizing the lens-to-sample distance and visualizing the sample's surface. The currently available data regarding fuel debris's elemental composition, distribution, shape, and size are still limited. These fuel debris data are crucial to deciding further strategies and decommissioning steps for the FDNPS. Additionally, a temperature gradient exists in the reactor vessels owing to the decay heat of the nuclear fuel debris. Therefore, investigating the effect of sample temperature and laser ablation angle (LAA) is crucial to adapt the system to in-situ measurements This talk will discuss the dependence of sample temperature and LAA on the laser-induced plasma-optical emission and LIP-acoustic signal for zirconium metal, which is a part of fuel debris.

口頭

Fiber-coupled acoustic wave-assisted microchip LIBS system for elemental composition and surface imaging of nuclear fuel debris

Batsaikhan, M.; 大場 弘則; 狩野 貴宏; 赤岡 克昭; 若井田 育夫

no journal, , 

In this invited talk, a brief discussion about fiber-coupled acoustic-wave assisted microchip LIBS (AW-mLIBS) system for elemental composition and surface imaging will be given.

口頭

革新的分光画像解析による燃料デブリの可視化への挑戦とLIBSによる検証,3; 遠隔操作LIBSによる元素マッピング

大場 弘則; Batsaikhan, M.; 赤岡 克昭; 狩野 貴宏; 岩田 圭弘; 若井田 育夫; 坂口 知聡*; 坂本 寛*; 牟田 浩明*

no journal, , 

福島第一原子力発電所(1F)炉内物質の分析手法として、ハイパースペクトルイメージング(HSI)とレーザー誘起ブレークダウン分光(LIBS)を組み合わせることを提案し、それぞれの分担において技術の適用性を検証している。東京電力福島第一原子力発電所の廃炉措置における燃料デブリ取出しに向けた位置・性状把握のための手段の一つとして、ファイバーLIBSによる遠隔その場分析が期待されている。しかしながら、LIBS技術において、対象物試料の元素分析を正しく行うためには、試料に対してパルスレーザー光を複数回照射して、プラズマ発光したときの信号強度を確認しながらレーザー光の焦点位置を調整する必要がある。そのため、焦点位置の調整の度に試料の表面が破壊されることや、本測定に至るまでの時間を要することなどが懸念される。今回、レーザー誘起音響波を利用してLIBS焦点位置の最適化を行い、同時に試料の2次元元素分布測定を試みた。その結果、音響波振幅の大きさと発光信号強度が一致し、分析に最適なレーザー光焦点位置を容易に決定することが可能となった。また、この方法を基礎にして多元素混合酸化物の組成分布が測定できることを実証した。

口頭

Two-dimensional elemental mapping of simulated fuel debris using laser induced breakdown spectroscopy

Batsaikhan, M.; 狩野 貴宏; 柴田 卓弥; 赤岡 克昭; 若井田 育夫

no journal, , 

Severe accident at Fukushima Daiichi Nuclear Power Station (1F) of Tokyo Electric Power Company Holdings (TEPCO) occurred after strong earthquake and massive tsunami. Since after the accident, many efforts to decommissioning of the 1F moving forward steadily and safely. It is important to realize a measurement technique that can distinguish fuel debris from other materials. In the present study, we focused on Laser Induced Breakdown Spectroscopy (LIBS) which is considered as a promising remote, in-situ and radiation tolerance technique for fuel debris inspection of the 1F. Although the LIBS is a point measurement technique, it has been used as elemental surface mapping technique in many fields, because it allows user to realize fast spatial scanning without any sample preparation. In this presentation, measurement result of 2D elemental mapping by LIBS on simulated fuel debris sample under atmospheric pressure and without radiation environment will be discussed.

口頭

Development of quick and remote analysis for severe accident reactor, 8-4; Development of acoustic-wave assisted microchip LIBS technique for simultaneous measurement of elemental mapping and surface recognition of nuclear fuel debris

Batsaikhan, M.; 大場 弘則; 狩野 貴宏; 赤岡 克昭; 若井田 育夫

no journal, , 

An acoustic-wave assisted microchip LIBS (AW-mLIBS) system was developed for simultaneous measurement of elemental mapping and surface recognition of fuel debris at the Fukushima Daiichi Nuclear Power Plant. In this presentation, an experimental study on the two-dimensional elemental mapping of Gadolinium (Gd) in a surrogate debris sample and surface imaging of the sample by the AW-mLIBS system will be presented.

口頭

A Laser-acoustic technique for simultaneous measurement of elemental and surface imaging of fuel debris

Batsaikhan, M.; 大場 弘則; 若井田 育夫

no journal, , 

Laser Induced Breakdown Spectroscopy (LIBS) technique has been considered a promising analytical technique for the elemental composition of fuel debris (including Gd-thermal neutron absorber in some fuel rods) formed inside reactor vessels at FDNPP. However, accurate controlling of the laser focusing position is important to create plasma on the sample surface and to achieve the best analytical performance when the LIBS technique is applied to the in-situ and on-site investigation of nuclear fuel debris at FDNPP where various targets having different sizes and shapes must be recognized and analyzed in a short time under high radiation environment. The objective of the present study is to develop a method for the simultaneous measurement of elemental distribution and surface imaging of nuclear fuel debris using acoustic wave-assisted microchip LIBS system.

口頭

Technology development for abbreviated (in-situ) analysis of fuel debris, 3; Demonstration of fiber-delivered LIBS for application to decommissioning sites, 2; LIBS performance evaluation using spent nuclear fuel.

Batsaikhan, M.; 大場 弘則*; 赤岡 克昭; 狩野 貴宏; 岩田 圭弘; 若井田 育夫*; 榮藤 良則*; 大内 敦*; 佐々 勝明*; 坂本 寛*

no journal, , 

福島第一廃炉措置における炉内外での核燃料物質遠隔分析を目指して光ファイバー伝送レーザー誘起ブレークダウン分光(ファイバーLIBS)装置を開発し、核燃料物質を含む試料への適用評価を進めている。今回は未照射U及びZr、Fe等を含有した試料を用いて検出下限値を評価するとともに、高線量率環境下での使用済燃料の2次元元素マッピングへの適用について紹介する。

口頭

燃料デブリの簡易(その場)分析のための技術開発,1; LIBSを用いた遠隔分析の概要

岩田 圭弘; 赤岡 克昭; 狩野 貴宏; Batsaikhan, M.; 大場 弘則*; 若井田 育夫*; 坂本 寛*; 中西 隆造*; 柏倉 俊介*; 出口 祥啓*; et al.

no journal, , 

福島第一原子力発電所の廃炉作業に向けて、燃料デブリ等の核燃料物質含有試料に対する遠隔分析として、レーザー誘起ブレークダウン分光法(LIBS)を用いた分析技術の開発を進めている。本講演では、LIBSを用いた遠隔分析の原理及び特徴を説明し、開発の進捗状況について紹介する。

口頭

燃料デブリの簡易(その場)分析のための技術開発,2; 現場適用を目指した光ファイバー伝送LIBS実証試験,1; 長距離および高放射線環境下での定量性評価

大場 弘則*; 中西 隆造*; Batsaikhan, M.; 若井田 育夫*

no journal, , 

福島第一廃炉措置における炉内外での核燃料物質遠隔分析を目指して光ファイバー伝送レーザー誘起ブレークダウン分光(ファイバーLIBS)装置を開発し、核燃料物質を含む試料への適用評価を進めている。汎用コネクタ接続による300m以上の超長尺分析の可能性を示すとともに、高放射線環境下でのマイクロチップレーザーLIBS分析特性を検量線から評価し、1kGy/hの高線量率環境でも変わらないことを実証した。

口頭

Laser-produced plasmas on metal Fe, Cu, and Zr in air, nitrogen, and argon at atmospheric pressure

Batsaikhan, M.; 大場 弘則

no journal, , 

Laser-induced breakdown spectroscopy allows us to perform remote and rapid measurements with little or no sample preparation. And also, there have been continuous efforts to apply LIBS to nuclear material analysis. In the current situation, the inside of the Fukushima Daiichi Nuclear Power Station is filled with nitrogen gas. This time, we report and discuss the results of the fundamental plasma characteristics of Cu, Fe, and Zr elements in ambient gas. Plasma emission formed at the Fe, Cu, and Zr metals in the air at atmospheric pressure was collected as a function of lens-to-sample distance. As an example, the resulting spectra of Fe, the strongest intensity from Fe, O, and N was observed at lens-to-sample distance = 0 and all measurements in the present work were performed at this position. We will discuss the plasma temperature of each element and gas.

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