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Journal Articles

Accelerator mass spectrometry of $$^{90}$$Sr in environmental samples utilizing laser photo-detachment

Honda, Maki; Martschini, M.*; Marchhart, O.*; Steier, P.*; Golser, R.*; Sakaguchi, Aya*

Hoshasen (Internet), 48(4), p.130 - 136, 2024/02

Strontium-90 ($$^{90}$$Sr, 28.9 years) is a key fission product nuclide in internal dose assessment because it accumulates in bones and teeth in the body, causing health problems. Therefore, it is essential to know the distribution of $$^{90}$$Sr in the environment and its temporal variation ($$^{90}$$Sr enrichment in biota), which requires efficient analysis of many environmental samples. An analysis of environmental samples with known $$^{90}$$Sr concentrations conducted with the 3 MV AMS facility (VERA: Vienna Environmental Research Accelerator) at the University of Vienna, Austria, towards the practical application of $$^{90}$$Sr AMS, the results of which are detailed in this paper. In this study, the validity of the AMS method was demonstrated by analyzing environmental samples with known $$^{90}$$Sr concentrations (IAEA-447, IAEA-A-12, and IAEA-TEL-2015-03 sample 5: 1 dry-g each). The chemical separation developed in this study takes approximately two days and is a more straightforward procedure than conventional $$beta$$-ray detection methods. The $$^{90}$$Sr measurements were conducted on the AMS system combined with the Ion Laser InterAction Mass Spectrometry (ILIAMS) system. The AMS method achieved a limit of detection $$<$$0.1 mBq ($$<$$ 1.3$$times$$10$$^{5}$$ atoms) for $$^{90}$$Sr, which is 1/30th of typical $$beta$$-ray detection. As a result of the lower detection limit, the AMS method allows $$^{90}$$Sr quantification with smaller sample volumes. For example, a Japanese freshwater sample with a $$^{90}$$Sr concentration of 4 mBq/L requires a sample volume of 5 liter

Journal Articles

Multiple mechanisms in proton-induced nucleon removal at $$sim$$100 MeV/nucleon

Pohl, T.*; Sun, Y. L.*; Obertelli, A.*; Lee, J.*; G$'o$mez-Ramos, M.*; Ogata, Kazuyuki*; Yoshida, Kazuki; Cai, B. S.*; Yuan, C. X.*; Brown, B. A.*; et al.

Physical Review Letters, 130(17), p.172501_1 - 172501_8, 2023/04

 Times Cited Count:5 Percentile:91.26(Physics, Multidisciplinary)

We report on the first proton-induced single proton- and neutron-removal reactions from the neutron deficient $$^{14}$$O nucleus with large Fermi-surface asymmetry at $$sim$$100 MeV/nucleon. Our results provide the first quantitative contributions of multiple reaction mechanisms including the quasifree knockout, inelastic scattering, and nucleon transfer processes. It is shown that the inelastic scattering and nucleon transfer, usually neglected at such energy regime, contribute about 50% and 30% to the loosely bound proton and deeply bound neutron removal, respectively.

Journal Articles

New measurement system based on small-angle neutron scattering for structural analysis of light-responsive materials

Iwase, Hiroki*; Akamatsu, Masaaki*; Inamura, Yasuhiro; Sakaguchi, Yoshifumi*; Morikawa, Toshiaki*; Kasai, Satoshi*; Ouchi, Keiichi*; Kobayashi, Kazuki*; Sakai, Hideki*

Journal of Applied Crystallography, 56(1), p.110 - 115, 2023/02

 Times Cited Count:2 Percentile:78.87(Chemistry, Multidisciplinary)

With the increasing importance of light-responsive materials, it is vital to analyze the relationship between function and structural changes induced by light irradiation. Small-angle scattering (SAS) is effective for such structural analysis. However, quantitatively capturing local molecular structure formation and molecular reactions at a scale of less than 1 nm via SAS is difficult. In this study, to analyze the structure of non-equilibrium phenomena in light-responsive materials, a new sample environment has been developed for a time-of-flight small- and wide-angle neutron scattering instrument (TAIKAN), comprising a UV-Vis irradiation system, UV-Vis absorption measurement equipment and photodetector. Simultaneous measurement of small-angle neutron scattering and UV-Vis absorption was achieved. This system was used to demonstrate the in situ observation of UV-Vis irradiation-induced structural change of micelles formed by a light-responsive surfactant sample in an aqueous solution.

Journal Articles

Challenging studies by accelerator mass spectrometry for the development of environmental radiology; Status report on the analysis of $$^{90}$$Sr and $$^{135}$$Cs by AMS

Honda, Maki; Martschini, M.*; Wieser, A.*; Marchhart, O.*; Lachner, J.*; Priller, A.*; Steier, P.*; Golser, R.*; Sakaguchi, Aya*

JAEA-Conf 2022-001, p.85 - 90, 2022/11

Accelerator mass spectrometry (AMS) is an analytical method that combines mass spectrometry with a tandem accelerator, which has been used mainly in nuclear physics experiments. AMS is used to measure radionuclides with half-lives of 10$$^{3}$$-10$$^{8}$$ years. For radionuclides with half-lives of this order, the method of measuring their mass is 10$$^{3}$$-10$$^{6}$$ times more sensitive than measuring their activity. Because of this advantage, AMS has been widely applied in Earth and planetary sciences, atomic energy research, and other fields. Among the various studies, Wallner et al. (2021, 2016) have achieved excellent work in Earth and planetary sciences. For example, they have attained the ultra-sensitive analysis of $$^{60}$$Fe and $$^{244}$$Pu in environmental samples. These are radionuclides produced by rapid-neutron-capture (r-process) nucleosynthesis. Our recent work shows that a new AMS system (VERA, University of Vienna), which combines laser isobaric separation and a typical AMS system, has been successfully applied to the ultra-sensitive determination of $$^{90}$$Sr and $$^{135}$$Cs in environment. For $$^{90}$$Sr in environmental samples, the $$beta$$-ray measurement by the milking of the daughter nuclide $$^{90}$$Y is still the principal method, which takes 3-6 weeks. The new AMS method has a detection limit of $$<$$ 0.1 mBq, which is comparable to that of $$beta$$-ray measurement, with a more straightforward chemical treatment than $$beta$$-measurement. Our achievement demonstrates that AMS can be a practical new method for determining $$^{90}$$Sr in the environment.

Journal Articles

Novel $$^{90}$$Sr analysis of environmental samples by ion-laser interaction mass spectrometry

Honda, Maki; Martschini, M.*; Marchhart, O.*; Priller, A.*; Steier, P.*; Golser, R.*; Sato, Tetsuya; Tsukada, Kazuaki; Sakaguchi, Aya*

Analytical Methods, 14(28), p.2732 - 2738, 2022/07

 Times Cited Count:2 Percentile:41.58(Chemistry, Analytical)

The sensitive $$^{90}$$Sr analysis with accelerator mass spectrometry (AMS) was developed for the advances of environmental radiology. One advantage of AMS is the ability to analyze various environmental samples with $$^{90}$$Sr/$$^{88}$$Sr atomic ratios of 10$$^{-14}$$ in a simple chemical separation. Three different IAEA samples with known $$^{90}$$Sr concentrations (moss-soil, animal bone, Syrian soil: 1 g each) were analyzed to assess the validity of the chemical separation and the AMS measurement. The $$^{90}$$Sr measurements were conducted on the AMS system combined with the Ion Laser InterAction MasSpectrometry (ILIAMS) setup at the University of Vienna, which has excellent isobaric separation performance. The isobaric interference of $$^{90}$$Zr in the $$^{90}$$Sr AMS was first removed by chemical separation. The separation factor of Zr in two-step column chromatography with Sr resin and anion exchange resin was 10$$^{6}$$. The $$^{90}$$Zr remaining in the sample was removed by ILIAMS effectively. This simple chemical separation achieved a limit of detection $$<$$ 0.1 mBq in the $$^{90}$$Sr AMS, which is lower than typical $$beta$$-ray detection. The agreement between AMS measurements and nominal values for the $$^{90}$$Sr concentrations of IAEA samples indicated that the new highly-sensitive $$^{90}$$Sr analysis in the environmental samples with AMS is reliable even for high matrix samples of soil and bone.

Journal Articles

Developing accelerator mass spectrometry capabilities for anthropogenic radionuclide analysis to extend the set of oceanographic tracers

Hain, K.*; Martschini, M.*; G$"u$lce, F.*; Honda, Maki; Lachner, J.*; Kern, M.*; Pitters, J.*; Quinto, F.*; Sakaguchi, Aya*; Steier, P.*; et al.

Frontiers in Marine Science (Internet), 9, p.837515_1 - 837515_17, 2022/03

 Times Cited Count:12 Percentile:95.78(Environmental Sciences)

Recent major advances in accelerator mass spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) regarding detection efficiency and isobar suppression have opened possibilities for the analysis of additional long-lived radionuclides at ultra-low environmental concentrations. These radionuclides, including $$^{233}$$U, $$^{135}$$Cs, $$^{99}$$Tc and $$^{90}$$Sr, will become important for oceanographic tracer application due to their generally conservative behavior in ocean water. In particular, the isotope ratios $$^{233}$$U/$$^{236}$$U and $$^{137}$$Cs/$$^{135}$$Cs have proven to be powerful fingerprints for emission source identification as they are not affected by elemental fractionation. Improved detection efficiencies allowed us to analyze all major long-lived actinides, i.e. $$^{236}$$U, $$^{237}$$Np, $$^{239, 240}$$Pu, $$^{241}$$Am as well as the very rare $$^{233}$$U, in the same 10 L water samples of an exemplary depth profile from the northwest Pacific Ocean. Especially for $$^{90}$$Sr analysis, our new approach has already been validated for selected reference materials (e.g. IAEA-A-12) and is ready for application in oceanographic studies. We estimate that a sample volume of only (1-3) L ocean water is sufficient for $$^{90}$$Sr as well as $$^{135}$$Cs analysis, respectively.

Journal Articles

First isolation and analysis of caesium-bearing microparticles from marine samples in the Pacific coastal area near Fukushima Prefecture

Miura, Hikaru*; Ishimaru, Takashi*; Ito, Yukari*; Kuribara, Yuichi; Otosaka, Shigeyoshi*; Sakaguchi, Aya*; Misumi, Kazuhiro*; Tsumune, Daisuke*; Kubo, Atsushi*; Higaki, Shogo*; et al.

Scientific Reports (Internet), 11, p.5664_1 - 5664_11, 2021/03

 Times Cited Count:13 Percentile:67.48(Multidisciplinary Sciences)

For the first time, we isolated and investigated seven CsMPs (radioactive caesium-bearing microparticles) from marine particulate matter and sediment. From the elemental composition, the $$^{134}$$Cs/$$^{137}$$Cs activity ratio, and the $$^{137}$$Cs activity per unit volume results, we inferred that the five CsMPs collected from particulate matter were emitted from Unit 2 of the FDNPP, whereas the two CsMPs collected from marine sediment were possibly emitted from Unit 3. The presence of CsMPs can cause overestimation of the solid-water distribution coefficient of Cs in marine sediments and particulate matter and a high apparent radiocaesium concentration factor for marine biota. CsMPs emitted from Unit 2, which were collected from the estuary of a river that flowed through a highly contaminated area, may have been deposited on land and then transported by the river. By contrast, CsMPs emitted from Unit 3 were possibly transported eastward by the wind and deposited directly onto the ocean surface.

Journal Articles

Quasifree neutron knockout reaction reveals a small $$s$$-Orbital component in the Borromean nucleus $$^{17}$$B

Yang, Z. H.*; Kubota, Yuki*; Corsi, A.*; Yoshida, Kazuki; Sun, X.-X.*; Li, J. G.*; Kimura, Masaaki*; Michel, N.*; Ogata, Kazuyuki*; Yuan, C. X.*; et al.

Physical Review Letters, 126(8), p.082501_1 - 082501_8, 2021/02

AA2020-0819.pdf:1.29MB

 Times Cited Count:45 Percentile:96.73(Physics, Multidisciplinary)

A quasifree ($$p$$,$$pn$$) experiment was performed to study the structure of the Borromean nucleus $$^{17}$$B, which had long been considered to have a neutron halo. By analyzing the momentum distributions and exclusive cross sections, we obtained the spectroscopic factors for $$1s_{1/2}$$ and $$0d_{5/2}$$ orbitals, and a surprisingly small percentage of 9(2)% was determined for $$1s_{1/2}$$. Our finding of such a small $$1s_{1/2}$$ component and the halo features reported in prior experiments can be explained by the deformed relativistic Hartree-Bogoliubov theory in continuum, revealing a definite but not dominant neutron halo in $$^{17}$$B. The present work gives the smallest $$s$$- or $$p$$-orbital component among known nuclei exhibiting halo features and implies that the dominant occupation of $$s$$ or $$p$$ orbitals is not a prerequisite for the occurrence of a neutron halo.

Journal Articles

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

Sasa, Kimikazu*; Honda, Maki; Hosoya, Seiji*; Takahashi, Tsutomu*; Takano, Kenta*; Ochiai, Yuta*; Sakaguchi, Aya*; Kurita, Saori*; Satou, Yukihiko; Sueki, Keisuke*

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

 Times Cited Count:8 Percentile:69.90(Nuclear Science & Technology)

Journal Articles

Characterization of two types of cesium-bearing microparticles emitted from the Fukushima accident via multiple synchrotron radiation analyses

Miura, Hikaru*; Kuribara, Yuichi; Yamamoto, Masayoshi*; Sakaguchi, Aya*; Yamaguchi, Noriko*; Sekizawa, Oki*; Nitta, Kiyofumi*; Higaki, Shogo*; Tsumune, Daisuke*; Itai, Takaaki*; et al.

Scientific Reports (Internet), 10, p.11421_1 - 11421_9, 2020/07

 Times Cited Count:18 Percentile:67.24(Multidisciplinary Sciences)

Journal Articles

How different is the core of $$^{25}$$F from $$^{24}$$O$$_{g.s.}$$ ?

Tang, T. L.*; Uesaka, Tomohiro*; Kawase, Shoichiro; Beaumel, D.*; Dozono, Masanori*; Fujii, Toshihiko*; Fukuda, Naoki*; Fukunaga, Taku*; Galindo-Uribarri, A.*; Hwang, S. H.*; et al.

Physical Review Letters, 124(21), p.212502_1 - 212502_6, 2020/05

 Times Cited Count:14 Percentile:72.90(Physics, Multidisciplinary)

The structure of a neutron-rich $$^{25}$$F nucleus is investigated by a quasifree ($$p,2p$$) knockout reaction. The sum of spectroscopic factors of $$pi 0d_{5/2}$$ orbital is found to be 1.0 $$pm$$ 0.3. The result shows that the $$^{24}$$O core of $$^{25}$$F nucleus significantly differs from a free $$^{24}$$O nucleus, and the core consists of $$sim$$35% $$^{24}$$O$$_{rm g.s.}$$, and $$sim$$65% excited $$^{24}$$O. The result shows that the $$^{24}$$O core of $$^{25}$$F nucleus significantly differs from a free $$^{24}$$O nucleus. The result may infer that the addition of the $$0d_{5/2}$$ proton considerably changes the neutron structure in $$^{25}$$F from that in $$^{24}$$O, which could be a possible mechanism responsible for the oxygen dripline anomaly.

Journal Articles

Difference in the solid-water distributions of radiocesium in rivers in Fukushima and Chernobyl

Takahashi, Yoshio*; Sakaguchi, Aya*; Fan, Q.*; Tanaka, Kazuya; Miura, Hikaru*; Kurihara, Yuichi*

Behavior of Radionuclides in the Environment I; Function of Particles in Aquatic System, p.115 - 150, 2020/00

 Times Cited Count:0 Percentile:0.59(Environmental Sciences)

Journal Articles

Repeatability and reproducibility of measurements of low dissolved radiocesium concentrations in freshwater using different pre-concentration methods

Kurihara, Momo*; Yasutaka, Tetsuo*; Aono, Tatsuo*; Ashikawa, Nobuo*; Ebina, Hiroyuki*; Iijima, Takeshi*; Ishimaru, Kei*; Kanai, Ramon*; Karube, Jinichi*; Konnai, Yae*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 322(2), p.477 - 485, 2019/11

 Times Cited Count:4 Percentile:40.00(Chemistry, Analytical)

We assessed the repeatability and reproducibility of methods for determining low dissolved radiocesium concentrations in freshwater in Fukushima. Twenty-one laboratories pre-concentrated three of 10 L samples by five different pre-concentration methods (prussian-blue-impregnated filter cartridges, coprecipitation with ammonium phosphomolybdate, evaporation, solid-phase extraction disks, and ion-exchange resin columns), and activity of radiocesium was measured. The z-scores for all of the $$^{137}$$Cs results were within $$pm$$2, indicating that the methods were accurate. The relative standard deviations (RSDs) indicating the variability in the results from different laboratories were larger than the RSDs indicating the variability in the results from each separate laboratory.

Journal Articles

Anomaly of structural relaxation in complex liquid metal of bismuth; Dynamic correlation function of coherent quasi-elastic neutron scattering

Kawakita, Yukinobu; Kikuchi, Tatsuya*; Inamura, Yasuhiro; Tahara, Shuta*; Maruyama, Kenji*; Hanashima, Takayasu*; Nakamura, Mitsutaka; Kiyanagi, Ryoji; Yamauchi, Yasuhiro*; Chiba, Kaori*; et al.

Physica B; Condensed Matter, 551, p.291 - 296, 2018/12

 Times Cited Count:11 Percentile:47.29(Physics, Condensed Matter)

There are elemental liquid metals with complex structures far from the hard sphere (HS) packing model. Liquid Bi has an asymmetric first peak in the structure factors S(Q). The pair distribution function g(r) exhibits strange distance ratio of 1:2 between the first and the second peaks. Since a HS model with two kinds of radius produces asymmetry of the main peak in S(Q), existence of short-lived covalent bonds was discussed. Contrarily, modulation of the atomic distribution by the Friedel oscillations of shielding electrons around metallic ions was discussed. To examine its bonding nature from viewpoints of dynamic correlation functions, we have measured neutron quasielastic scattering of liquid Bi by using cold disk chopper spectrometer installed at MLF of J-PARC. The van Hove function revealed that the shoulder structure located at a longer side of the first peak in g(r) exhibits a longer relaxation time than the main structures such as the first and second peaks.

Journal Articles

Kinetics of silver photodiffusion into amorphous Ge$$_{20}$$S$$_{80}$$ films; Case of pre-reaction

Sakaguchi, Yoshifumi*; Hanashima, Takayasu*; Aoki, Hiroyuki; Asaoka, Hidehito; Simon, A.-A. A.*; Mitkova, M.*

Physica Status Solidi (A), 215(12), p.1800049_1 - 1800049_12, 2018/06

 Times Cited Count:6 Percentile:29.80(Materials Science, Multidisciplinary)

Journal Articles

Discovery of radiocesium-bearing microparticles in river water and their influence on the solid-water distribution coefficient ($$K_{rm d}$$) of radiocesium in the Kuchibuto River in Fukushima

Miura, Hikaru*; Kurihara, Yuichi*; Sakaguchi, Aya*; Tanaka, Kazuya; Yamaguchi, Noriko*; Higaki, Shogo*; Takahashi, Yoshio*

Geochemical Journal, 52(2), p.145 - 154, 2018/00

 Times Cited Count:50 Percentile:94.06(Geochemistry & Geophysics)

Solid-water distribution coefficient ($$K_{rm d}$$) of radiocesium in rivers is apparently increased due to the possible presence of highly radioactive radiocesium-bearing microparticles (CsMPs) in the solid phase. In this study, we evaluated the contribution of CsMPs to apparent Kd values. The ratio of the radioactivity of the separated CsMPs to the total radiocesium on fluvial suspended particles ranged from 0 to 46%. This means that the existence of CsMPs in fluvial suspended partcles did not change apparent Kd values in order magnitude.

Journal Articles

Mineralogical control of the size distribution of stable Cs and radiocesium in riverbed sediments

Tanaka, Kazuya; Watanabe, Naoko*; Yamasaki, Shinya*; Sakaguchi, Aya*; Fan, Q.*; Takahashi, Yoshio*

Geochemical Journal, 52(2), p.173 - 185, 2018/00

 Times Cited Count:9 Percentile:42.40(Geochemistry & Geophysics)

We analyzed riverbed sediments collected at two sites, Yamakiya and Kuroiwa, in Fukushima after the Fukushima accident. The size distributions of K, Rb, and $$^{133}$$Csreflected the mineralogy of sediments, where primary host minerals for these alkali elements would be biotite, K-feldspar, and clay minerals. Silt-size fractions contained high $$^{133}$$Cs and $$^{137}$$Cs concentrations possibly due to adsorption on clay minerals. Their concentrations decreased with particle size at the Yamakiya site. In contrast, coarse and very coarse sand fractions from the Kuroiwa site showed higher $$^{133}$$Cs and $$^{137}$$Cs concentrations in comparison to fine - medium sand fractions. The coarse sand fractions contained many weathered biotite grains. Overall, the size distributions of $$^{133}$$Cs and $$^{137}$$Cs were similar in the sediments, suggesting that the Fukushima-derived radiocesium was distributed into each particle size fraction in response to the distribution of the stable Cs that was controlled by mineralogical composition.

Journal Articles

Estimation of desorption ratios of radio/stable caesium from environmental samples (aerosols and soils) leached with seawater, diluted seawater and ultrapure water

Sakaguchi, Aya*; Chiga, Haruka*; Tanaka, Kazuya; Tsuruta, Haruo*; Takahashi, Yoshio*

Geochemical Journal, 52(2), p.187 - 199, 2018/00

 Times Cited Count:7 Percentile:34.60(Geochemistry & Geophysics)

An aerosol sample collected on the 15th of March 2011 at Kawasaki City (Kanagawa) was sequentially leached with seawater for 30 days. As a result, about 60% of the total $$^{137}$$Cs was extracted. In addition, a surface soil sample collected from Kawamata Town (Fukushima) two months after the Fukushima accident, was leached for 223 days with a natural seawater, a 1:1 mixture of ultrapure water and seawater, and ultrapure water. Eventually, more than 15% of the total $$^{137}$$Cs in the surface soil sample was efficiently desorbed by seawater leaching. In comparison, about 9% of the total $$^{137}$$Cs was leached with 1:1 diluted seawater and less than 1% of the total $$^{137}$$Cs was leached with ultrapure water over the 223 days. Overall, $$^{133}$$Cs and $$^{137}$$Cs showed similar leaching behaviour.

Journal Articles

Comparison of solid-water partitions of radiocesium in river waters in Fukushima and Chernobyl Areas

Takahashi, Yoshio*; Fan, Q.*; Suga, Hiroki*; Tanaka, Kazuya; Sakaguchi, Aya*; Takeichi, Yasuo*; Ono, Kanta*; Mase, Kazuhiko*; Kato, Kenji*; Kanivets, V. V.*

Scientific Reports (Internet), 7(1), p.12407_1 - 12407_11, 2017/09

 Times Cited Count:28 Percentile:67.53(Multidisciplinary Sciences)

We focused on factors controlling partition of radiocesium on particulate matters and sediments in rivers of Fukushima and Chernobyl. Radiocesium is more soluble in the Pripyat River (Chernobyl) due to weaker interaction of radiocesium with clay minerals caused by the inhibition effect of the adsorbed humic substances. In contrast, particulate matters and sediments in the Kuchibuto River (Fukushima) display high adsorption affinity with lesser inhibition effect of adsorbed humic substances. This difference is possibly governed by the geology and soil type of provenances surrounding both catchments.

Journal Articles

Summary of study on environmental radioactivity effected from the accident at the TEPCO Fukushima Daiichi Nuclear Power Plant in 5 years after the accident

Iimoto, Takeshi*; Kinoshita, Norikazu*; Sakaguchi, Aya*; Sugihara, Shinji*; Takamiya, Koichi*; Tagami, Keiko*; Nagao, Seiya*; Bessho, Kotaro*; Matsumura, Hiroshi*; Miura, Taichi*; et al.

KEK Report 2016-3, 134 Pages, 2017/03

This report is summary of study on environmental radioactivity effected from the accident at the TEPCO Fukushima Daiichi Nuclear Power Plant in 5 years after the accident. It was compiled efforts related to the accident reported from the 13th to the 17th "Workshop on Environmental Radioactivity" which was held at the High Energy Accelerator Research and Development Organization.

111 (Records 1-20 displayed on this page)