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Atmospheric resuspension of insoluble radioactive cesium bearing particles found in the difficult-to-return area in Fukushima

Tang, P.*; 北 和之*; 五十嵐 康人*; 佐藤 志彦; 畑中 恒太郎*; 足立 光司*; 木名瀬 健*; 二宮 和彦*; 篠原 厚*

Progress in Earth and Planetary Science (Internet), 9(1), p.17_1 - 17_15, 2022/03

 被引用回数:3 パーセンタイル:66.57(Geosciences, Multidisciplinary)

The deposition of insoluble radiocesium bearing microparticles (CsMPs), which were released from the Fukushima Daiichi Nuclear Power Plant (F1NPP) accident in March 2011, has resulted in the widespread contamination of eastern Japan. Obviously, these deposited insoluble CsMPs may become the secondary contamination sources by atmospheric migration or other environmental transferring process, however, the understanding of the transport mechanism remains non-elucidation, and the relevant evidence has not been directly provided. This study, for the first time, provides the direct evidence for the resuspension of these insoluble CsMPs to the atmosphere from (1) proximity of $$^{137}$$Cs radioactivity and resemblance of the morphology and the elemental compositions of CsMPs in the samples of soil and aerosol derived from the same sampling site, (2) the special characteristics of the resuspended CsMPs of which the ratios of Na/Si, K/Si and/or Cs/Si were smaller than those from the initially released CsMPs collected at either long distance or near F1NPP, which can be ascribed to the slowly natural corrosion of CsMPs by the loss of the small amount of soluble contents in CsMPs, and (3) high CsMPs concentration of 10 granules/gram in the surface soil of our sampling site, and high resuspension frequency of CsMPs in spring when predominant suspended particles were soil dust.


Inflammatory signaling and DNA damage responses after local exposure to an insoluble radioactive microparticle

松谷 悠佑; 浜田 信行*; 谷内 淑恵*; 佐藤 志彦; 石川 正純*; 伊達 広行*; 佐藤 達彦

Cancers (Internet), 14(4), p.1045_1 - 1045_15, 2022/02

 被引用回数:7 パーセンタイル:86.13(Oncology)

福島原子力発電所の事故後、不溶性の放射性セシウム含有微粒子(Cs-BMP)が発見された。放射性Cs摂取後の内部被ばくのリスクに関しては、従来、可溶性Csが全身へ均一に分布した条件を想定した臓器線量から推定されてきた。一方、Cs-BMPは正常組織に長期的に付着し、慢性的な不均一被ばくを引き起こす可能性がある。本研究では、Cs-BMPによる不均一被ばく後の放射線影響の解明へ向けて、炎症応答とDNA損傷誘発との関係を調査した。炎症性シグナル経路であるNF-$$kappa$$B p65とCOX-2に焦点を当てた実験により、$$gamma$$線による均一被ばくと比較して、Cs-BMPの近位の細胞ではNF-$$kappa$$B p65が活性化される一方、遠位の細胞ではNF-$$kappa$$B p65と同時にCOX-2も有意に活性化する傾向を観察した。また、炎症性シグナルの阻害剤を用いた実験により、Cs-BMP近位の細胞の放射線感受性の低下と遠位の細胞の放射線感受性の増強の双方に対し、炎症性シグナルの活性が深く関与することがわかった。これらの結果は、Cs-BMPによる被ばく後の放射線影響は、従来の均一被ばくに基づく推定とは異なることを示唆している。


Odd-parity autoionizing levels of uranium observed by two-color two-step photoionization optogalvanic spectroscopy

宮部 昌文; 佐藤 志彦; 若井田 育夫; 寺林 稜平*; Sonnenschein, V.*; 富田 英生*; Zhao, Y.*; 坂本 哲夫*

Journal of Physics B; Atomic, Molecular and Optical Physics, 54(14), p.145003_1 - 145003_8, 2021/07

 被引用回数:0 パーセンタイル:0.01(Optics)



Deposition and dispersion of radio-cesium released due to the Fukushima Nuclear accident, 2; Sensitivity to aerosol microphysical properties of Cs-bearing microparticles (CsMPs)

梶野 瑞王*; 足立 光司*; 五十嵐 康人*; 佐藤 志彦; 澤田 壮弘*; 関山 剛*; 財前 祐二*; 佐谷 茜*; 鶴田 治雄*; 森口 祐一*

Journal of Geophysical Research; Atmospheres, 126(1), p.e2020JD033460_1 - e2020JD033460_23, 2021/01

 被引用回数:11 パーセンタイル:75.36(Meteorology & Atmospheric Sciences)

The dispersion and deposition of radio-cesium ($$^{137}$$Cs) carried by the two types (type A and type B) of water-insoluble Cs-bearing solid microparticles (CsMPs) released due to the Fukushima nuclear accident were simulated for the first time. The presence of type B CsMPs (70-400 $$mu$$m found in soil and 1-5 $$mu$$m found in air), associated with the hydrogen explosion of Unit 1 in the afternoon of March 12, could partly explain the simulated underestimation of total deposition over land by assuming that 100% of the Cs carriers were water-soluble submicron particles (WSPs). Type A CsMPs (0.1-10 $$mu$$m), released from Units 2 or 3 in the midnight between March 14 and 15, travelled over the Kanto Plain, the most populated plain in Japan. Differences in the size distribution of type A CsMPs altered the surface air concentration over Kanto substantially, by up to more than one order of magnitude. The major deposition mechanisms varied among dry, wet, and fog depositions depending on the size distribution. The simulated activity fractions due to the CsMPs in the total deposition were compared to those observed in surface soil for the first time. The observations could be explained by the simulations for the locations under the influence of type B CsMPs. However, the simulations were substantially underestimated for the locations influenced by type A CsMPs. There could be more fractions of type A CsMPs emission in the source term and/or the simulated deposition rates of type A CsMPs were underestimated.


A Sensitive method for Sr-90 analysis by accelerator mass spectrometry

笹 公和*; 本多 真紀; 細谷 青児*; 高橋 努*; 高野 健太*; 落合 悠太*; 坂口 綾*; 栗田 沙緒里*; 佐藤 志彦; 末木 啓介*

Journal of Nuclear Science and Technology, 58(1), p.72 - 79, 2021/01

 被引用回数:8 パーセンタイル:73.58(Nuclear Science & Technology)

Strontium-90 ($$^{90}$$Sr) is one of the most important fission products due to the potential health risks of its uptake and retention in the human body. Conventional analysis techniques involve beta-counting, which requires ingrowth of $$^{90}$$Y over a period of two weeks or more. Accelerator mass spectrometry (AMS) has the potential to shorten the analysis time while offering a lower limit of detection than beta-counting. Here, Sr in samples was recovered as SrF$$_{2}$$ to provide sufficient negative ions in the caesium-sputtering ion source. In the sample preparation step, 95-98% of Sr was recovered and 99-100% of Zr removed by ion-exchange separation. Sr recovery was $$sim$$30% in the precipitation process, and this can be improved. The recovered $$^{90}$$Sr was mixed with PbF$$_{2}$$ at an SrF$$_{2}$$:PbF$$_{2}$$ weight ratio of 4:1. A maximum 500 nA beam current of Sr$$_{3}$$ ions was obtained from SrF$$_{2}$$ samples. A five-anode gas ionization detector was used to avoid isobaric interference from $$^{90}$$Zr. The $$^{90}$$Sr/Sr atomic ratio background of $$sim$$6 $$times$$ 10$$^{-13}$$ (equivalent to $$sim$$3 mBq $$^{90}$$Sr) was comparable with that achieved at other AMS facilities. Good linearity $$^{90}$$Sr/Sr atomic ratios was obtained from 1.75 $$times$$ 10$$^{-10}$$ to 3.38 $$times$$ 10$$^{-9}$$. Suitable techniques for sample preparation and measurement were thus achieved for $$^{90}$$Sr analysis by AMS.


Structural and compositional characteristics of Fukushima release particulate material from Units 1 and 3 elucidates release mechanisms, accident chronology and future decommissioning strategy

Martin, P. G.*; Jones, C. P.*; Bartlett, S.*; Ignatyev, K.*; Megson-Smith, D.*; 佐藤 志彦; Cipiccia, S.*; Batey, D. J.*; Rau, C.*; 末木 啓介*; et al.

Scientific Reports (Internet), 10, p.22056_1 - 22056_17, 2020/12

 被引用回数:1 パーセンタイル:7.6(Multidisciplinary Sciences)

The structural form and elemental distribution of material originating from different Fukushima Daiichi Nuclear Power Plant reactors (Units 1 and 3) is hereby examined to elucidate their contrasting release dynamics and the current in-reactor conditions to influence future decommissioning challenges. Complimentary computed X-ray absorption tomography and X-ray fluorescence data show that the two suites of Si-based material sourced from the different reactor Units have contrasting internal structure and compositional distribution. The known event and condition chronology correlate with the observed internal and external structures of the particulates examined, which suggest that Unit 1 ejecta material sustained a greater degree of melting than that likely derived from reactor Unit 3. In particular, we attribute the near-spherical shape of Unit 1 ejecta and their internal voids to there being sufficient time for surface tension to round these objects before the hot (and so relatively low viscosity) silicate melt cooled to form glass. In contrast, a more complex internal form associated with the sub-mm particulates invoked to originate from Unit 3 suggest a lower peak temperature, over a longer duration. Using volcanic analogues, we consider the structural form of this material and how it relates to its environmental particulate stability and the bulk removal of residual materials from the damaged reactors. We conclude that the brittle and angular Unit 3 particulate are more susceptible to further fragmentation and particulate generation hazard than the round, higher-strength, more homogenous Unit 1 material.


Project IPAD; A Database to catalogue the analysis of Fukushima Daiichi accident fragmental release material

Martin, P.*; Alhaddad, O.*; Verbelen, Y.*; 佐藤 志彦; 五十嵐 康人*; Scott, T. B.*

Scientific Data (Internet), 7, p.282_1 - 282_8, 2020/08

 被引用回数:2 パーセンタイル:16.07(Multidisciplinary Sciences)

The 2011 accident at Japan's Fukushima Daiichi Nuclear Power Plant released a considerable inventory of radioactive material into the local and global environments. While the vast majority of this contamination was in the form of gaseous and aerosol species, of which a large component was distributed out over the neighbouring Pacific Ocean (where is was subsequently deposited), a substantial portion of the radioactive release was in particulate form and was deposited across Fukushima Prefecture. To provide an underpinning understanding of the dynamics of this catastrophic accident, alongside assisting in the off-site remediation and eventual reactor decommissioning activities, the "International Particle Analysis Database", or "IPAD", was established to serve as an interactive repository for the continually expanding analysis dataset of the sub-mm ejecta particulate. In addition to a fully interrogatable database of analysis results for registered users (exploiting multiple search methods), the database also comprises an open-access front-end for members of the public to engage with the multi-national analysis activities by exploring a streamlined version of the data.


Assessment of the mode of occurrence and radiological impact of radionuclides in Nigerian coal and resultant post-combustion coal ash using scanning electron microscopy and gamma-ray spectroscopy

Okeme, I. C.*; Scott, T. B.*; Martin, P. G.*; 佐藤 志彦; Ojonimi, T. I.*; Olaluwoye, M. O.*

Minerals (Internet), 10(3), p.241_1 - 241_15, 2020/03

 被引用回数:4 パーセンタイル:43.51(Geochemistry & Geophysics)

Natural radionuclide concentrations in coal and associated fly ash can occur at levels well in excess of those observed in other materials; enough to raise potential human and environmental health concerns when (re)suspended or incorporated into construction materials. To evaluate such concerns, this study characterised coal and fly ash samples obtained from two Nigerian coal mines (Okaba and Omelewu) using high resolution gamma spectroscopy combined with scanning electron microscopy and energy dispersive spectroscopy. Discrete uraninite particles were observed dispersed within the fly ash samples, alongside U and Th containing mineral grains (monazite, xenotime and zircon) with monazite the most abundant radioactive mineral particles. The pitted and cracked surface morphologies of these radioactive particles (with sizes between 10$$mu$$m and 80$$mu$$m) indicates their susceptibility for disintegration into more dangerous and readily inhalable PM2.5 aerosol particles, with the potential to deliver localised dose and cause chronic respiratory diseases. While the results of activity concentrations and radiological hazard indices (radium equivalent, annual effective dose equivalent, total radium, and excess lifetime cancer risk) from Okaba and Omelewu coal samples were of no concern, results for the corresponding fly ash samples from both mines were between 3 and 5 times higher than internationally recommended safe limits. These results therefore imply that such coal-derived fly ash is not safe for incorporation in the construction of residential houses and should be properly disposed of or contained to prevent hazard due to increased risk of prolonged indoor exposure to gamma radiation, radon gas and inhalation of liberated radioactive particles.


Compositional and structural analysis of Fukushima-derived particulates using high-resolution X-ray imaging and synchrotron characterisation techniques

Martin, P. G.*; Jones, C. P.*; Cipiccia, S.*; Batey, D. J.*; Hallam, K. R.*; 佐藤 志彦; Griffiths, I.*; Rau, C.*; Richards, D. A.*; 末木 啓介*; et al.

Scientific Reports (Internet), 10(1), p.1636_1 - 1636_11, 2020/01

 被引用回数:7 パーセンタイル:36.59(Multidisciplinary Sciences)

Both the three-dimensional internal structure and elemental distribution of near-field radioactive fallout particulate material released during the March 2011 accident at the Fukushima Daiichi Nuclear Power Plant is analysed using combined high-resolution laboratory and synchrotron radiation X-ray techniques. Results from this study allow for the proposition of the likely formation mechanism of the particles, as well as the potential risks associated with their existence in the environment, and the likely implications for future planned reactor decommissioning. A suite of particles is analyzed from a locality 2 km from the north-western perimeter of the site north of the primary contaminant plume in an area formerly attributed to being contaminated by fallout from reactor Unit 1. The particles are shown to exhibit significant structural similarities; being amorphous with a textured exterior, and containing inclusions of contrasting compositions, as well as an extensive internal void volume bimodal in its size distribution. A heterogeneous distribution of the various elemental constituents is observed inside a representative particle, which also exhibited a Fukushima-derived radiocesium ($$^{134}$$Cs, $$^{135}$$Cs and $$^{137}$$Cs) signature with negligible natural Cs. We consider the structure and composition of the particle to suggest it formed from materials associated with the reactor Unit 1 building explosion, with debris fragments embedded into the particles surface. Such a high void ratio, comparable to geological pumice, suggests such material formed during a rapid depressurisation and is potentially susceptible to fragmentation through attrition.


Pre- and post-accident $$^{14}$$C activities in tree rings near the Fukushima Dai-ichi Nuclear Power Plant

松中 哲也*; 笹 公和*; 高橋 努*; 松村 万寿美*; 佐藤 志彦; Shen, H.*; 末木 啓介*; 松崎 浩之*

Radiocarbon, 61(6), p.1633 - 1642, 2019/12

 被引用回数:2 パーセンタイル:12.08(Geochemistry & Geophysics)

Areas affected by routine radiocarbon ($$^{14}$$C) discharges from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) and accidental releases in March 2011 were investigated by analysis of cores from Japanese cypress and cedar trees growing at sites 9 and 24 km northwest of the plant. $$^{14}$$C concentrations in tree rings from 2008-2014 (before and after the accident) were determined by accelerator mass spectrometry, with $$^{14}$$C activities in the range 231-256 Bq kg$$^{-1}$$ C. Activities during the period 2012-2014, after FDNPP shutdown, represent background levels, while the significantly higher levels recorded during 2008-2010, before the accident, indicate uptake of $$^{14}$$C from routine FDNPP operations. The mean excess $$^{14}$$C activity for the pre-accident period at the sites 9 and 24 km northwest of the plant were 21 and 12 Bq kg$$^{-1}$$ C, respectively, indicating that the area of influence during routine FDNPP operations extended at least 24 km northwest. The mean excess tree-ring $$^{14}$$C activities in 2011 were 10 and 5.8 Bq kg$$^{-1}$$ C at 9 and 24 km northwest, respectively, documenting possible impact of the FDNPP accident on $$^{14}$$C levels in trees.



五十嵐 淳哉*; Zhang, Z. J.*; 二宮 和彦*; 篠原 厚*; 佐藤 志彦; 箕輪 はるか*; 吉川 英樹

KEK Proceedings 2019-2, p.54 - 59, 2019/11



A Review of Cs-bearing microparticles in the environment emitted by the Fukushima Dai-ichi Nuclear Power Plant accident

五十嵐 康人*; 小暮 敏博*; 栗原 雄一; 三浦 輝*; 奥村 大河*; 佐藤 志彦; 高橋 嘉夫*; 山口 紀子*

Journal of Environmental Radioactivity, 205-206, p.101 - 118, 2019/09

 被引用回数:60 パーセンタイル:71.65(Environmental Sciences)

福島第一原子力発電所事故ではチェルノブイリ原発事故と異なるケイ素,酸素,鉄,亜鉛を含む放射性微粒子が発見された。この放射性微粒子は高濃度のセシウムを含むことからセシウムマイクロパーティクル(CsMP)と呼ばれることもある。またこの粒子は少なくとも2種類が見つかっており、発見された順番に、2, 3号機(放出源未確定)と1号機由来をそれぞれTypeA, TypeBと呼んでおり、Cs同位体比, 形態, 採取場所で分類されている。本レビューではこれらの背景を含むCsMPの全体像を紹介する。


Formation of radioactive cesium microparticles originating from the Fukushima Daiichi Nuclear Power Plant accident; Characteristics and perspectives

大貫 敏彦*; 佐藤 志彦; 宇都宮 聡*

Journal of Nuclear Science and Technology, 56(9-10), p.790 - 800, 2019/09

 被引用回数:9 パーセンタイル:63.81(Nuclear Science & Technology)

Following the identification of radioactive particulates, particularly Cs microparticles (CsMPs) in aerosol samples collected on 14-15 March 2011 at Tsukuba, $$sim$$ 170 km south of the Fukushima Daiichi Nuclear Power Plant (FDNPP), numerous reports on CsMPs have been published. This paper reviews recent progress in the measurement and characterization of CsMPs by advanced analytical techniques, including advanced transmission electron microscopy (TEM) and synchrotron X-ray analysis. These analyses revealed that the CsMPs contained Si, Fe, Zn, Cs, and minor quantities of U together with some fission products. Uranium in the CsMPs was identified as being in the form of uraninite and (U,Zr)O$$_{2}$$. Detailed advanced TEM analysis has clarified some of the processes resulting in alteration of constituents of the nuclear fuels and containment vessel materials during this severe accident. In addition, the Tokyo Electric Power Company in cooperation with the Japan Atomic Energy Agency and the International Research Institute for Nuclear Decommissioning issued a detailed report on the elemental compositions and structures of the fuel debris fragments collected inside and outside of the primary containment vessel. This report highlighted the fact that the fuel debris fragments contained nanoparticles with the U and Zr components having similar structures to that of the CsMPs. This similarity in structures has stimulated further research on the structure and elemental constituents, especially for U and Zr in the CsMPs, and has opened up new avenues for studying the chemical characteristics of the fuel debris.


First determination of Pu isotopes ($$^{239}$$Pu, $$^{240}$$Pu and $$^{241}$$Pu) in radioactive particles derived from Fukushima Daiichi Nuclear Power Plant accident

五十嵐 淳哉*; Zheng, J.*; Zhang, Z.*; 二宮 和彦*; 佐藤 志彦; 福田 美保*; Ni, Y.*; 青野 辰雄*; 篠原 厚*

Scientific Reports (Internet), 9(1), p.11807_1 - 11807_10, 2019/08

 被引用回数:19 パーセンタイル:66.82(Multidisciplinary Sciences)



DNA damage induction during localized chronic exposure to an insoluble radioactive microparticle

松谷 悠佑; 佐藤 志彦; 浜田 信行*; 伊達 広行*; 石川 正純*; 佐藤 達彦

Scientific Reports (Internet), 9(1), p.10365_1 - 10365_9, 2019/07

 被引用回数:12 パーセンタイル:63.7(Multidisciplinary Sciences)

不溶性放射性微粒子(Cs含有粒子)は、呼吸器系に吸引された後、長期にわたって気管に付着し、微粒子周辺の正常組織に不均一な線量分布をもたらすと考えられている。このような微粒子によってもたらされる生物影響は不明なままであるため、本研究では、均一な被ばくとの比較の中で、微粒子による局所的慢性被ばく下において蓄積される核内DNA損傷を研究した。我々は、微粒子を含むマイクロキャピラリーを、正常肺細胞を含む培養皿に配置し、24時間もしくは48時間被ばく後に核内誘発$$gamma$$-H2AX focusの有意な変化を観察した。モンテカルロ計算と均一被ばくとの比較から、微粒子による局所被ばく下では、遠位細胞に対する細胞間シグナル誘発DNA損傷と近位細胞に対するDNA損傷誘発の低減(防御効果)の両者が誘発されることが示唆された。微粒子による臓器線量は微量であることから、従来の放射線リスク評価で十分であると思われる。本研究により、不溶性Cs含有粒子による不均一暴露下でのDNA損傷の空間分布を定量化することに初めて成功した。


Provenance of uranium particulate contained within Fukushima Daiichi Nuclear Power Plant Unit 1 ejecta material

Martin, P. G.*; Louvel, M.*; Cipiccia, S.*; Jones, C. P.*; Batey, D. J.*; Hallam, K. R.*; Yang, I. A. X.*; 佐藤 志彦; Rau, C.*; Mosselmans, J. F. W.*; et al.

Nature Communications (Internet), 10, p.2801_1 - 2801_7, 2019/06

 被引用回数:24 パーセンタイル:78.93(Multidisciplinary Sciences)



福島第一事故由来物質に対する環境モニタリング手法の最先端,1; 福島第一原発事故で放出した放射性粒子

佐藤 志彦

日本原子力学会誌ATOMO$$Sigma$$, 61(6), p.446 - 448, 2019/06

福島第一原子力発電所事故では大量の放射性物質が環境中に放出したが、チェルノブイリ原子力発電所事故のような炉心が直に大気と触れるような事象は発生しなかったため、核燃料を主とした放射性粒子の放出はないものと考えられていた。しかし2013年以降、放射性セシウム(Cs)を取込んだケイ素が主成分の微粒子が報告され、Cs-bearing particle、不溶性セシウム粒子などの名称で放射性粒子の存在が認知されるようになった。本稿では不溶性セシウム粒子がなぜ不思議な存在であるか、そしてどうして福島第一原子力発電所の廃炉で重要かを紹介した。


Activity of $$^{90}$$Sr in fallout particles collected in the difficult-to-return zone around the Fukushima Daiichi Nuclear Power Plant

Zhang, Z.*; 五十嵐 淳哉*; 佐藤 志彦; 二宮 和彦*; 末木 啓介*; 篠原 厚*

Environmental Science & Technology, 53(10), p.5868 - 5876, 2019/05

 被引用回数:19 パーセンタイル:64.97(Engineering, Environmental)




太田 祐貴*; 末木 啓介*; 笹 公和*; 高橋 努*; 松中 哲也*; 松村 万寿美*; 戸崎 裕貴*; 本多 真紀*; 細谷 青児*; 高野 健太*; et al.

JAEA-Conf 2018-002, p.99 - 102, 2019/02

福島第一原子力発電所事故により放出された放射性核種に長寿命の$$^{36}$$Cl(半減期: 30.1万年)がある。$$^{36}$$Clは放射性廃棄物の処理の際に土壌中における高い移動能と相まって重要な核種である。しかし、土壌中では無機塩素(Clinorg)が有機塩素(Clorg)に変換・保持されることで、その移動の機構は不明である。本研究では、汚染地域の無機$$^{36}$$Clの深度分布を得ることで$$^{36}$$Clの動態を検討し、事故による$$^{36}$$Cl汚染の程度を検討した。また、5cm表土に含まれる$$^{36}$$Clについても検討した。2017年における深度分布では、$$^{36}$$Cl濃度は表層で最も高くなり、深度とともに緩やかに減少した。一方で、$$^{36}$$Cl/Clはほぼ一定(平均値: 3.24$$pm$$0.55 ($$times$$10$$^{-12}$$))の値を示した。事故前の$$^{36}$$Cl/Clと比べると$$^{36}$$Cl/Clの増加を示し、事故由来の$$^{36}$$Clは土壌3.6g/cm$$^{2}$$(=5cm深)より深く移動していることが分かった。


Radiocarbon variations in tree rings since 1960 near the Tokai nuclear facility, Japan

松中 哲也*; 笹 公和*; 高橋 努*; 細谷 青児*; 松村 万寿美*; 佐藤 志彦; Shen, H.*; 末木 啓介*

Nuclear Instruments and Methods in Physics Research B, 439, p.64 - 69, 2019/01

 被引用回数:2 パーセンタイル:23.69(Instruments & Instrumentation)


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