Hydrogen vibration excitations of ZrH and TiH up to 21 GPa by incoherent inelastic neutron scattering

Hattori, Takanori; Nakamura, Mitsutaka; Iida, Kazuki*; Machida, Akihiko*; Sano, Asami; Machida, Shinichi*; Arima, Hiroshi*; Oshita, Hidetoshi*; Honda, Takashi*; Ikeda, Kazutaka*; et al.

Physical Review B, 106(13), p.134309_1 - 134309_9, 2022/10

https://doi.org/10.1103/PhysRevB.106.134309

Hydrogen vibration excitations of fluorite-type ZrH and TiH were investigated up to 21 GPa and 4 GPa, respectively, by incoherent inelastic neutron scattering experiments. The first excitation energies increased with pressure, as described by the equations (meV) = 141.4(2) + 1.02(2)(GPa) and (meV) = 149.4(1) + 1.21(8)(GPa) for ZrH and TiH, respectively. Coupling with pressure dependence of lattice parameters, the relations between metal-hydrogen distance () and are found to be well described by the equations (meV) = 1.62(9) 10 ((meV) = 1.47(21) 10 (AA), respectively. The slopes of these curves are much steep compared to the previously reported trend in various fluorite-type metal hydrides at ambient pressure. The hydrogen wave function spreading showed that the local potential field for a hydrogen atom shrinks more intensively than the tetrahedral site. These behavior is likely caused by the rigid metal ion core and the resulting confinement of the hydrogen atom in the narrower potential field at high pressures.

Observation of dihydrogen bonds in high-pressure phases of ammonia borane by X-ray and neutron diffraction measurements

Nakano, Satoshi*; Sano, Asami; Hattori, Takanori; Machida, Shinichi*; Komatsu, Kazuki*; Fujihisa, Hiroshi*; Yamawaki, Hiroshi*; Goto, Yoshito*; Kikegawa, Takumi*

Inorganic Chemistry, 60(5), p.3065 - 3073, 2021/03

https://doi.org/10.1021/acs.inorgchem.0c03345

X-ray and neutron diffraction analyses of ammonia borane were conducted at ambient and high pressures. The H-H distance in dihydrogen bonds was shorter than twice the van der Waals radius (2.4 ). The half of the dihydrogen bonds were broken on phase transition from AP to the first high pressure phase (HP1) at approximately 1.2 GPa as revealed by an increase in the H-H distances. On further pressure increase, all of the H-H distances became shorter than 2.4 again, implying the pressure-induced reformation of the dihydrogen bonds. Furthermore, the HP1 transformed to the second one with the structure of (Z = 2) at about 11 GPa. In this phase transition, the inclination of the molecule axis became larger and the number of types of dihydrogen bonds increased from 6 to 11. Just before the third transition at 18.9 GPa, the shortest dihydrogen bond decreased to 1.65 . The present study experimentally first confirmed the breakage and reformation of the dihydrogen bonds by the structural change under pressure.

Status of study of long-term assessment of transport of radioactive contaminants in the environment of Fukushima (FY2018) (Translated document)

Nagao, Fumiya; Niizato, Tadafumi; Sasaki, Yoshito; Ito, Satomi; Watanabe, Takayoshi; Dohi, Terumi; Nakanishi, Takahiro; Sakuma, Kazuyuki; Hagiwara, Hiroki; Funaki, Hironori; et al.

JAEA-Research 2020-007, 249 Pages, 2020/10

JAEA-Research-2020-007.pdf:15.83MB

The accident of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. occurred due to the Great East Japan Earthquake, Sanriku offshore earthquake, of 9.0 magnitude and the accompanying tsunami. As a result, large amount of radioactive materials was released into the environment. Under these circumstances, Japan Atomic Energy Agency (JAEA) has been conducting "Long-term Assessment of Transport of Radioactive Contaminants in the Environment of Fukushima" concerning radioactive materials released in environment, especially migration behavior of radioactive cesium since November 2012. This report is a summary of the research results that have been obtained in environmental dynamics research conducted by JAEA in Fukushima Prefecture.

Practical effects of pressure-transmitting media on neutron diffraction experiments using Paris-Edinburgh presses

Hattori, Takanori; Sano, Asami; Machida, Shinichi*; Ouchi, Keiichi*; Kira, Hiroshi*; Abe, Jun*; Funakoshi, Kenichi*

High Pressure Research, 40(3), p.325 - 338, 2020/09

https://doi.org/10.1080/08957959.2020.1782899

To understand the practical effects of pressure-transmitting media (PTM) on neutron diffraction using Paris-Edinburgh presses, diffraction patterns of MgO were collected to approximately 20 GPa using PTMs of Pb, AgCl, 4:1 methano-ethanol (ME) mixture with and without heating, N, and Ar. Hydrostaticity in the sample chamber estimated from the MgO 220 peak width improves in the order of Pb, AgCl, Ar, ME mixture, N, and the heated ME mixture. Unlike previous results using a diamond anvil cell, the unheated ME mixture is superior to Ar even after freezing, probably due to the cup on the anvil face. Considering these results and the sizable coherent scattering of Ne, which would show good hydrostaticity, we conclude that the ME mixture (preferably the heated one) is the best PTM in neutron experiments up to 20 GPa, while Ar can be substituted when a sample is reactive to alcohols.

Simulation study of the effects of buildings, trees and paved surfaces on ambient dose equivalent rates outdoors at three suburban sites near Fukushima Dai-ichi

Kim, M.; Malins, A.; Yoshimura, Kazuya; Sakuma, Kazuyuki; Kurikami, Hiroshi; Kitamura, Akihiro; Machida, Masahiko; Hasegawa, Yukihiro*; Yanagi, Hideaki*

Journal of Environmental Radioactivity, 210, p.105803_1 - 105803_10, 2019/12

https://doi.org/10.1016/j.jenvrad.2018.09.001

To improve the accuracy of simulations for air dose rates over fallout contaminated areas, the distribution of the radionuclides within the environment should be modelled realistically, e.g. considering differences in radioactivity levels between agricultural land, urban surfaces, and forest compartments. Moreover simulations should model the shielding of rays by buildings, trees and land topography. Here we outline a system for generating three dimensional models of urban and rural areas in Fukushima Prefecture. The Cs and Cs radioactivity distribution can be set flexibly across the different components of the model. The models incorporate realistic representations of local buildings, based on nine common Japanese designs, individual conifer and broadleaf trees, and the topography of the land surface. Models are generated from Digital Elevation Model (DEM) and Digital Surface Model (DSM) datasets, and refined by users assisted with ortho-photographs of target sites. Completed models are exported from the system in a format suitable for the Particle and Heavy Ion Transport code System (PHITS) for the calculation of air dose rates and other radiological quantities. The system is demonstrated by modelling a suburban area 4 km from the Fukushima Daiichi Nuclear Power Plant that has yet to be decontaminated. Air dose rates calculated in PHITS were correlated with measurements taken across the site in a car-borne survey.

Long-term simulations of radiocesium discharge in watershed with improved radiocesium wash-off model; Applying the model to Abukuma River basin of Fukushima

Liu, X.; Machida, Masahiko; Kurikami, Hiroshi; Kitamura, Akihiro

Journal of Environmental Radioactivity, 203, p.135 - 146, 2019/07

https://doi.org/10.1016/j.jenvrad.2019.03.001

In order to simulate the long-term migration and distribution of radiocesium after the Fukushima accident, a numerical model, Soil and Cesium Transport (SACT) based on universal soil loss equation (USLE), has been developed in previous studies. Although the SACT model's results on radiocesium discharge in 2011 are in reasonable agreement with field measurements, it fails to capture the sharp decrease of radiocesium flux in subsequent years, especially in the case of Abukuma River. We therefore have improved SACT by implementing the vertical migration and fixation of radiocesium in soil. For validation purpose, the annual average radiocesium concentration in sediments discharged from Abukuma River has been evaluated from measurement data. New model achieved much better agreement with the measurement results without parameter tuning.

Modelling the effect of mechanical remediation on dose rates above radiocesium contaminated land

Malins, A.; Kurikami, Hiroshi; Kitamura, Akihiro; Machida, Masahiko

Remediation Measures for Radioactively Contaminated Areas, p.259 - 272, 2019/00

https://doi.org/10.1007/978-3-319-73398-2_12

Pair distribution function analysis of nanostructural deformation of calcium silicate hydrate under compressive stress

Bae, S.*; Jee, H.*; Kanematsu, Manabu*; Shiro, Ayumi*; Machida, Akihiko*; Watanuki, Tetsu*; Shobu, Takahisa; Suzuki, Hiroshi

Journal of the American Ceramic Society, 101(1), p.408 - 418, 2018/01

https://doi.org/10.1111/jace.15185

Despite enormous interest in calcium silicate hydrate (C-S-H), its detailed atomic structure and intrinsic deformation under an external load are lacking. This study demonstrates the nanostructural deformation process of C-S-H in tricalcium silicate (CS) paste as a function of applied stress by interpreting atomic pair distribution function (PDF) based on in situ X-ray scattering. Three different strains in CS paste under compression were compared using a strain gauge and the real and reciprocal space PDFs. PDF refinement revealed that the C-S-H phase mostly contributed to PDF from 0 to 20 whereas crystalline phases dominated that beyond 20. The short-range atomic strains exhibited two regions for C-S-H: I) plastic deformation (0-10 MPa) and II) linear elastic deformation (10 MPa), whereas the long-range deformation beyond 20 was similar to that of Ca(OH). Below 10 MPa, the short-range strain was caused by the densification of C-S-H induced by the removal of interlayer or gel-pore water. The strain is likely to be recovered when the removed water returns to C-S-H.

Characteristics of radio-cesium transport and discharge between different basins near to the Fukushima Dai-ichi Nuclear Power Plant after heavy rainfall events

Sakuma, Kazuyuki; Kitamura, Akihiro; Malins, A.; Kurikami, Hiroshi; Machida, Masahiko; Mori, Koji*; Tada, Kazuhiro*; Kobayashi, Takamaru*; Tawara, Yasuhiro*; Tosaka, Hiroyuki*

Journal of Environmental Radioactivity, 169-170, p.137 - 150, 2017/04

https://doi.org/10.1016/j.jenvrad.2016.12.006

This paper describes watershed modeling of catchments surrounding the Fukushima Dai-ichi Nuclear Power Plant to understand radio-cesium redistribution by water flows and sediment transport. We extended our previously developed three-dimensional hydrogeological model of the catchments to calculate the migration of radio-cesium in both sediment-sorbed and dissolved forms. The simulations cover the entirety of 2013, including nine heavy rainfall events, as well as Typhoon Roke in September 2011. Typhoons Man-yi and Wipha were the strongest typhoons in 2013 and had the largest bearing on radio-cesium redistribution. The simulated Cs discharge quantities over the nine events in 2013 are in good agreement with field monitoring observations. Deposition mainly occurs on flood plains and points where the river beds broaden in the lower basins, and within dam reservoirs along the rivers. Differences in Cs discharge ratios between the five basins are explained by differences in the initial fallout distribution within the basins, the presence of dam reservoirs, and the input supply to watercourses. It is possible to use these simulation results to evaluate future radioactive material distributions in order to support remediation planning.

Redistribution and export of contaminated sediment within eastern Fukushima Prefecture due to typhoon flooding

Kitamura, Akihiro; Kurikami, Hiroshi; Sakuma, Kazuyuki; Malins, A.; Okumura, Masahiko; Machida, Masahiko; Mori, Koji*; Tada, Kazuhiro*; Tawara, Yasuhiro*; Kobayashi, Takamaru*; et al.

Earth Surface Processes and Landforms, 41(12), p.1708 - 1726, 2016/09

https://doi.org/10.1002/esp.3944

Sediment erosion and transport processes that are considered to be important in predicting the future radioactive material distribution through sediment-sorbed form in Fukushima Prefecture are simulated. Since large portion of the sediment is considered to be supplied into the rivers, it is important to trace their migration process in terms of each river basin. We choose five river basins, namely the Odaka, the Ukedo, the Maeda, the Kuma, and the Tomioka, from north to south, because of their importance in contamination aspects and prediction studies. The results are summarized as comprehensive dataset of sediment migration for particular river basins in typical typhoon events that account for the most of annual soil erosion. Detail calculations implemented for the amount of sediment supplied in to the river, deposited on river and dam beds, and exported to the ocean.