A Decade of neutron diffraction study of iron hydrides

Aoki, Katsutoshi*; Machida, Akihiko*; Saito, Hiroyuki*; Hattori, Takanori

Koatsuryoku No Kagaku To Gijutsu, 35(1), p.4 - 11, 2025/03

https://doi.org/10.4131/jshpreview.35.4

Iron reacts with hydrogen to form solid solutions with body-centered cubic, face-centered cubic, hexagonal close packed, and double hexagonal close packed structures at high temperatures and high pressures. Neutron diffraction is the most powerful tool for determining the occupation sites and occupancies of hydrogen atoms dissolved in a metal lattice. Structural parameters, including hydrogen occupation sites and occupancies, are refined via Rietveld analysis for neutron diffraction data. We present our expertise in Rietveld refinement of iron hydrides accumulated over 10 years.

Imaging Josephson vortices on curved junctions

Fujisawa, Yuita*; Krishnadas, A*; Nakamura, Tomonori*; Hsu, C.-H.*; Smith, B. R. M.*; Pardo-Almanza, M*; Hiyane, Hoshu*; Nagai, Yuki; Machida, Tadashi*; Okada, Yoshinori*

Physical Review B, 110(22), p.224511_1 - 224511_5, 2024/12

https://doi.org/10.1103/PhysRevB.110.224511

Understanding the nature of vortices in type-II superconductors has been vital for deepening the physics of exotic superconductors and applying superconducting materials to future electronic devices. A recent study has shown that the LiTiO(111) thin film offers a unique experimental platform to unveil the nature of the vortex along the curved Josephson junction. This study successfully visualized individual Josephson vortices along the curved Josephson junctions using in-situ spectroscopic scanning tunneling microscopy on LiTiO (111) epitaxial thin films. Notably, the local curvature of the Josephson junction was discovered to control the position of Josephson vortices. Furthermore, the numerical simulation reproduces the critical role of the curvature of the Josephson junction. This study provides guidelines to control Josephson vortices through geometrical ways, such as mechanical controlling of superconducting materials and their devices.

Addendum: Site occupancy of interstitial deuterium atoms in face-centred cubic iron

Machida, Akihiko*; Saito, Hiroyuki*; Sugimoto, Hidehiko*; Hattori, Takanori; Sano, Asami; Endo, Naruki*; Katayama, Yoshinori*; Iizuka, Riko*; Sato, Toyoto*; Matsuo, Motoaki*; et al.

Nature Communications (Internet), 15, p.8861_1 - 8861_2, 2024/10

https://doi.org/10.1038/s41467-024-52736-1

In our previous article (Nature Commun. 5, 5063 (2014)), the site occupancies of D atoms dissolved in an fcc Fe metal lattice were investigated via Rietveld refinement of neutron powder diffraction patterns collected at 988 K and 6.3 GPa. The fcc metal lattice has two interstitial sites available for accommodating D atoms: octahedral and tetrahedral sites. The Rietveld refinement revealed that D atoms occupied mainly the octahedral sites with occupancy of 0.532 and slightly the tetrahedral sites with occupancy of 0.056. Subsequent density-functional-theory (DFT) calculations by Antonov (Phys. Rev. Mater. 2019)) showed that the occupation energy on the tetrahedral site was significantly higher than that on the octahedral site; the tetrahedral site occupation was unlikely to occur even at temperatures as high as 988 K. We reexamined the site occupancies of D-atom by Rietveld refinement including extinction correction. As a result, the octahedral occupancy was increased to 0.60 and the tetrahedral occupancy was reduced to zero. The occupation of only the octahedral site for D atom is consistent with the DFT calculation, although in contrast to the previous results.

Hydroxyl group/fluorine disorder in deuterated magnesium hydroxyfluoride and behaviors of hydrogen bonds under high pressure

He, X.*; Kagi, Hiroyuki*; Komatsu, Kazuki*; Iizuka, Riko*; Okajima, Hajime*; Hattori, Takanori; Sano, Asami; Machida, Shinichi*; Abe, Jun*; Goto, Hirotada*; et al.

Journal of Molecular Structure, 1310, p.138271_1 - 138271_8, 2024/08

https://doi.org/10.1016/j.molstruc.2024.138271

High-pressure responses of the O-DF hydrogen bonds in deuterated magnesium hydroxyfluoride were investigated using neutron powder diffraction and Raman spectroscopy. The Rietveld analysis at ambient conditions revealed a chemical formula of Mg(OD)F and hydroxyl group/fluorine disorder (OD/F disorder) in the crystal structure, which gave rise to two hydrogen-bonding configurations. The Rietveld analysis showed the hydrogen-bonding geometries remains up to 9.8 GPa, indicating no pressure-induced strengthening of hydrogen bonds. The Raman spectra at ambient conditions showed three hydroxyl stretching bands at 2613, 2694, and 2718 cm. The high frequencies of the O-D stretching modes indicated that the hydroxyls should be involved in weak or none hydrogen-bonding interactions. Up to 20.2 GPa, the mode initially centered at 2694 cm displayed a pressure-induced blue shift, revealing no strengthening of hydrogen bonds under compression. We discuss the existence of hydrogen bonds and the causes of the blue-shifting hydroxyls at ambient and at high pressures.

Hydrogen bond symmetrisation in DO ice observed by neutron diffraction

Komatsu, Kazuki*; Hattori, Takanori; Klotz, S.*; Machida, Shinichi*; Yamashita, Keishiro*; Ito, Hayate*; Kobayashi, Hiroki*; Irifune, Tetsuo*; Shimmei, Toru*; Sano, Asami; et al.

Nature Communications (Internet), 15, p.5100_1 - 5100_7, 2024/06

https://doi.org/10.1038/s41467-024-48932-8

Hydrogen bond symmetrisation is the phenomenon where a hydrogen atom is located at the centre of a hydrogen bond. Theoretical studies predict that hydrogen bonds in ice VII eventually undergo symmetrisation upon increasing pressure, involving nuclear quantum effect with significant isotope effect and drastic changes in the elastic properties through several intermediate states with varying hydrogen distribution. Despite numerous experimental studies conducted, the location of hydrogen and hence the transition pressures reported up to date remain inconsistent. Here we report the atomic distribution of deuterium in DO ice using neutron diffraction above 100 GPa and observe for the first time the transition from a bimodal to a unimodal distribution of deuterium at around 80 GPa. At the transition pressure, a significant narrowing of the peak widths of 110 was also observed, attributed to the structural relaxation by the change of elastic properties.

Simulation of predicted effects of decontamination and cultivation activities on reduction of air dose rates using Monte Carlo method

Kim, M.; Yoshimura, Kazuya; Sakuma, Kazuyuki; Malins, A.*; Abe, Tomohisa; Nakama, Shigeo; Machida, Masahiko; Saito, Kimiaki

Kankyo Hoshano Josen Gakkai-Shi, 12(2), p.39 - 53, 2024/04

More than ten years have passed since the accident at TEPCO's Fukushima Daiichi Nuclear Power Station. But with the progress of decontamination, the evacuation order has been lifted and the return of residents is still ongoing. Under these circumstances, in order to quantitatively evaluate the effect of decontamination activities and cultivation on air dose rate reduction, a detailed environmental model was constructed using 3D-ADRES for a real area located in the Okuma town, Fukushima prefecture. Monte Carlo simulations were performed using the model to calculate realistic distributions of radioactive Cs based on measurement results and air dose rates reflecting changes over time. As a result, the distribution of air dose rates at 100 cm above ground level in the target area according to decontamination and cultivation activities was calculated. The calculated air dose rates reproduced the measured values well, and were confirmed to be appropriate as a method for evaluating the effects of decontamination and cultivation activities. This method is expected to serve as a reference for further decontamination management measures to reduce the air dose rate in the difficult-to-return zone, where entry is still restricted.

Neutron transmission CB-KID imager using samples placed at room temperature

Ishida, Takekazu*; Vu, TheDang*; Shishido, Hiroaki*; Aizawa, Kazuya; Oku, Takayuki; Oikawa, Kenichi; Harada, Masahide; Kojima, Kenji M*; Miyajima, Shigeyuki*; Koyama, Tomio*; et al.

Journal of Low Temperature Physics, 214(3-4), p.152 - 157, 2024/02

https://doi.org/10.1007/s10909-023-03030-9

Estimation of temporal variation of discharged inventory of radioactive strontium Sr (Sr) from port of Fukushima Daiichi Nuclear Power Plant; Analysis of the temporal variation from the accident to March 2022 and evaluation of its impact on Fukushima coast and offshore areas

Machida, Masahiko; Iwata, Ayako; Yamada, Susumu; Otosaka, Shigeyoshi*; Kobayashi, Takuya; Funasaka, Hideyuki*; Morita, Takami*

Nihon Genshiryoku Gakkai Wabun Rombunshi (Internet), 22(4), p.119 - 139, 2023/11

https://doi.org/10.3327/taesj.J22.016

We estimate monthly discharged inventory of Sr from port of Fukushima Daiichi Nuclear Power Plant (1F) from Jun. 2013 to Mar. 2022 by using the Voronoi tessellation method inside the port, following the monitoring of Sr sea water radioactivity concentration inside the port. The results suggest that the closure of sea side impermeable wall is the most effective for the reduction of discharged one. In addition, the results roughly reveal the monthly discharged inventory required to observe visible enhancement of the sea radioactivity concentration from the background level in each area. Such outcome is significant for considering environmental impacts on the planned future releasing of the treated water accumulated in 1F site.

Inverse estimation scheme of radioactive source distributions inside building rooms based on monitoring air dose rates using LASSO; Theory and demonstration

Shi, W.*; Machida, Masahiko; Yamada, Susumu; Yoshida, Toru*; Hasegawa, Yukihiro*; Okamoto, Koji*

Progress in Nuclear Energy, 162, p.104792_1 - 104792_19, 2023/08

https://doi.org/10.1016/j.pnucene.2023.104792

Predicting radioactive source distributions inside reactor building rooms based on monitoring air dose rates is one of the most essential steps towards decommissioning of nuclear power plants. However, the attempt is rather a difficult task, because it can be generally mapped onto mathematically ill-posed problem. Then, in order to successfully perform the inverse estimations on radioactive source distributions even in such ill-posed conditions, we suggest that a machine learning method, least absolute shrinkage and selection operator (LASSO) minimizing the loss function, is a promising scheme. For the purpose of its feasibility demonstrations in real building rooms, we employ PHITS code to make LASSO input as the above matrix C connecting the radioactive source vector P defined on surface meshes of structural materials with the air dose rate vector Q measured at internal positions inside the rooms. We develop a mathematical criterion on the number of monitoring points to correctly predict source distributions based on the theory of Candes and Tao. Then, we confirm that LASSO actually shows extremely high possibility for source distribution reconstructions as far as the number of detection points satisfies our criterion. Moreover, we verify that radioactive hot spots can be truly reconstructed in an experiment setup. At last, we examine an influence factor like detector-source distance to enhance the predicting possibility in the inverse estimation. From the above demonstrations, we propose that LASSO scheme is a quite useful way to explore hot spots as seen in damaged nuclear power plants like Fukushima Daiichi nuclear power plants.

LASSO reconstruction scheme for radioactive source distributions inside reactor building rooms with spectral information and multi-radionuclide contaminated situations

Shi, W.*; Machida, Masahiko; Yamada, Susumu; Yoshida, Toru*; Hasegawa, Yukihiro*; Okamoto, Koji*

Annals of Nuclear Energy, 184, p.109686_1 - 109686_12, 2023/05

https://doi.org/10.1016/j.anucene.2023.109686