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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
High-pressure responses of the O-D
F 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.
neutron diffractionKobayashi, Hiroki*; Komatsu, Kazuki*; Ito, Hayate*; Machida, Shinichi*; Hattori, Takanori; Kagi, Hiroyuki*
Journal of Physical Chemistry Letters (Internet), 14(47), p.10664 - 10669, 2023/11
Times Cited Count：1 Percentile：0.01(Chemistry, Physical)Ice IV is a metastable high-pressure phase of ice in which the water molecules exhibit orientational disorder. Although orientational ordering is commonly observed for other ice phases, it has not been reported for ice IV. We conducted powder neutron diffraction experiments for DCl-doped D
O ice IV to investigate hydrogen ordering in ice IV. We found abrupt changes in the temperature derivative of unit cell volume, dV/dT, at about 120 K, and revealed their slightly ordered structure at low temperatures based on the Rietveld method. The occupancy of the D1 site deviates from 0.5; it increased when samples were cooled at higher pressures and reached 0.282(5) at 2.38 GPa, 58 K. Our results evidence the presence of a low-symmetry hydrogen-ordered state corresponding to ice IV. It seems, however, difficult to experimentally access the completely ordered phase corresponding to ice IV by slow cooling at high pressure.
Yamashita, Keishiro*; Nakayama, Kazuya*; Komatsu, Kazuki*; Ohara, Takashi; Munakata, Koji*; Hattori, Takanori; Sano, Asami; Kagi, Hiroyuki*
Acta Crystallographica Section B; Structural Science, Crystal Engineering and Materials (Internet), 79(5), p.414 - 426, 2023/10
Times Cited Count：0 Percentile：0.02(Chemistry, Multidisciplinary)The structure of a recently-found hyperhydrated form of sodium chloride, NaCl
13H(D)O, has been determined by single-crystal neutron diffraction at 1.7 GPa and 298 K. It has large hydrogen-bond networks and some water molecules have distorted bonding features such as bifurcated hydrogen bonds and five-coordinated water molecules. The hydrogen-bond network has similarities to ice VI in terms of network topology and disordered hydrogen bonds. Assuming the equivalence of network components connected by pseudo symmetries, the overall network structure of this hydrate can be expressed by breaking it down into smaller structural units which correspond to the ice VI network structure. This hydrogen-bond network contains orientational disorder of water molecules in contrast to the known salt hydrates. Here, we present an example for further insights into a hydrogen-bond network containing ionic species.
Ni
D
at high 
conditionsShito, Chikara*; Kagi, Hiroyuki*; Kakizawa, Sho*; Aoki, Katsutoshi*; Komatsu, Kazuki*; Iizuka, Riko*; Abe, Jun*; Saito, Hiroyuki*; Sano, Asami; Hattori, Takanori
American Mineralogist, 108(4), p.659 - 666, 2023/04
Times Cited Count：1 Percentile：59.64(Geochemistry & Geophysics)The phase relation and crystal structure of FeNiH (D) at high pressures and temperatures up to 12 GPa and 1000 K were clarified by in-situ X-ray and neutron diffraction measurements. Under conditions of the present study, no deuterium atoms occupied tetragonal (
) sites of face-centered cubic (fcc) FeNiD unlike fcc FeH(D). The deuterium-induced volume expansion per deuterium 
was determined as 2.45(4) 
and 3.31(6) for fcc and hcp phases, respectively, which were significantly larger than the corresponding values for FeD. The value slightly increased with increasing temperature. This study suggests that only 10% of nickel in iron drastically changes the behaviors of hydrogen in metal. Assuming that is constant regardless of pressure, the maximum hydrogen content in the Earth's inner core is estimated to be one to two times the amount of hydrogen in the oceans.
Nakada, Akira; Kanai, Katsuta; Kokubun, Yuji; Nagaoka, Mika; Koike, Yuko; Yamada, Ryohei*; Kubota, Tomohiro; Hirao, Moe; Yoshii, Hideki*; Otani, Kazunori*; et al.
JAEA-Review 2022-079, 116 Pages, 2023/03
JAEA-Review-2022-079.pdf:2.77MB
Based on the regulations (the safety regulation of Tokai Reprocessing Plant, the safety regulation of nuclear fuel material usage facilities, the radiation safety rule, the regulation about prevention from radiation hazards due to radioisotopes, which are related with the nuclear regulatory acts, the local agreement concerning with safety and environment conservation around nuclear facilities, the water pollution control law, and by law of Ibaraki Prefecture), the effluent control of liquid waste discharged from the Nuclear Fuel Cycle Engineering Laboratories of Japan Atomic Energy Agency has been performed. This report describes the effluent control results of the liquid waste in the fiscal year 2021. In this period, the concentrations and the quantities of the radioactivity in liquid waste discharged from the reprocessing plant, the plutonium fuel fabrication facilities, and the other nuclear fuel material usage facilities were much lower than the limits authorized by the above regulations.
FeO
solid solutions under high-pressure and high-temperature conditionsYamanaka, Takamitsu*; Hirao, Naohisa*; Nakamoto, Yuki*; Mikouchi, Takashi*; Hattori, Takanori; Komatsu, Kazuki*; Mao, H.-K.*
Physics and Chemistry of Minerals, 49(10), p.41_1 - 41_14, 2022/10
Times Cited Count：0 Percentile：0.02(Materials Science, Multidisciplinary)Magnetic and crystal structure of MnFeO solid solutions under high-PT conditions are investigated by neutron diffraction and synchrotron M
ssbauer spectroscopy. The ferrimagnetic-paramagnetic transition and tetragonal-cubic transition of Mn
FeO spinel occur at 100
C and 180C, respectively, suggesting both the transitions are not coupled. The structure transition temperature decreases with pressure. Mssbauer experiments and neutron diffraction revealed that the Fe
occupancy in tetrahedral site increases increase with pressure, suggesting MnFeO phase approaches inverse spinel. Magnetic structure refinement clarified paramagnetic and ferrimagnetic structure of MnFeO and MnFeO. These spinels transform into high-pressure orthorhombic phases at 18.4 and 14.0 GPa, respectively, indicating lower transition pressure with increasing Mn content.
Yamashita, Keishiro*; Komatsu, Kazuki*; Klotz, S.*; Fabelo, O.*; Fern
ndez-D
az, M. T.*; Abe, Jun*; Machida, Shinichi*; Hattori, Takanori; Irifune, Tetsuo*; Shimmei, Toru*; et al.
Proceedings of the National Academy of Sciences of the United States of America, 119(40), p.e2208717119_1 - e2208717119_6, 2022/10
Times Cited Count：2 Percentile：20.4(Multidisciplinary Sciences)Here we present the first elucidation of the disordered structure of ice VII, the dominant high-pressure form of water, at 2.2 GPa and 298 K from both single-crystal and powder neutron diffraction techniques. We reveal the three-dimensional atomic distributions from the maximum entropy method and unexpectedly find a ring-like distribution of hydrogen in contrast to the commonly-accepted discrete sites. In addition, total scattering analysis at 274 K clarified the difference in the intermolecular structure from ice VIII, the ordered counterpart of ice VII, despite an identical molecular geometry. Our complementary structure analyses robustly demonstrate the unique disordered structure of ice VII. Furthermore, these noble findings are related to the proton dynamics which drastically vary with pressure, and will contribute to an understanding of the structural origin of anomalous physical properties of ice VII under pressures.
Komatsu, Yuya*; Shimizu, Ryota*; Sato, Ryuhei*; Wilde, M.*; Nishio, Kazunori*; Katase, Takayoshi*; Matsumura, Daiju; Saito, Hiroyuki*; Miyauchi, Masahiro*; Adelman, J. R.*; et al.
Chemistry of Materials, 34(8), p.3616 - 3623, 2022/04
Times Cited Count：9 Percentile：76.65(Chemistry, Physical)Yamashita, Keishiro*; Komatsu, Kazuki*; Ohara, Takashi; Munakata, Koji*; Irifune, Tetsuo*; Shimmei, Toru*; Sugiyama, Kazumasa*; Kawamata, Toru*; Kagi, Hiroyuki*
High Pressure Research, 42(1), p.121 - 135, 2022/03
Times Cited Count：3 Percentile：56.47(Physics, Multidisciplinary)Nakano, Masanao; Nakada, Akira; Kanai, Katsuta; Nagaoka, Mika; Koike, Yuko; Yamada, Ryohei; Kubota, Tomohiro; Yoshii, Hideki*; Otani, Kazunori*; Hiyama, Yoshinori*; et al.
JAEA-Review 2021-040, 118 Pages, 2021/12
JAEA-Review-2021-040.pdf:2.48MB
Based on the regulations (the safety regulation of Tokai Reprocessing Plant, the safety regulation of nuclear fuel material usage facilities, the radiation safety rule, the regulation about prevention from radiation hazards due to radioisotopes, which are related with the nuclear regulatory acts, the local agreement concerning with safety and environment conservation around nuclear facilities, the water pollution control law, and by law of Ibaraki Prefecture), the effluent control of liquid waste discharged from the Nuclear Fuel Cycle Engineering Laboratories of Japan Atomic Energy Agency has been performed. This report describes the effluent control results of the liquid waste in the fiscal year 2020. In this period, the concentrations and the quantities of the radioactivity in liquid waste discharged from the reprocessing plant, the plutonium fuel fabrication facilities, and the other nuclear fuel material usage facilities were much lower than the limits authorized by the above regulations.
Kumazoe, Hiroyuki*; Igarashi, Yasuhiko*; Iesari, F.*; Shimizu, Ryota*; Komatsu, Yuya*; Hitosugi, Taro*; Matsumura, Daiju; Saito, Hiroyuki*; Iwamitsu, Kazunori*; Okajima, Toshihiko*; et al.
AIP Advances (Internet), 11(12), p.125013_1 - 125013_5, 2021/12
Times Cited Count：2 Percentile：17.05(Nanoscience & Nanotechnology)Ouchi, Kazuki; Komatsu, Atsushi; Takao, Koichiro*; Kitatsuji, Yoshihiro; Watanabe, Masayuki
Chemistry Letters, 50(6), p.1169 - 1172, 2021/06
Times Cited Count：2 Percentile：14.19(Chemistry, Multidisciplinary)The electrochemical behavior of uranium (IV) tetrachloride in ionic liquid-DMF mixture was studied for first time in order to build a redox flow battery (RFB) using U as an electrode active material. We found a quasi-reversible U
/U
couple that could be applied to the anode reaction of the RFB.
Kitazato, Kohei*; Milliken, R. E.*; Iwata, Takahiro*; Abe, Masanao*; Otake, Makiko*; Matsuura, Shuji*; Takagi, Yasuhiko*; Nakamura, Tomoki*; Hiroi, Takahiro*; Matsuoka, Moe*; et al.
Nature Astronomy (Internet), 5(3), p.246 - 250, 2021/03
Times Cited Count：44 Percentile：97.1(Astronomy & Astrophysics)Here we report observations of Ryugu's subsurface material by the Near-Infrared Spectrometer (NIRS3) on the Hayabusa2 spacecraft. Reflectance spectra of excavated material exhibit a hydroxyl (OH) absorption feature that is slightly stronger and peak-shifted compared with that observed for the surface, indicating that space weathering and/or radiative heating have caused subtle spectral changes in the uppermost surface. However, the strength and shape of the OH feature still suggests that the subsurface material experienced heating above 300 
C, similar to the surface. In contrast, thermophysical modeling indicates that radiative heating does not increase the temperature above 200 C at the estimated excavation depth of 1 m, even if the semimajor axis is reduced to 0.344 au. This supports the hypothesis that primary thermal alteration occurred due to radiogenic and/or impact heating on Ryugu's parent body.
Nakano, Masanao; Fujii, Tomoko; Nagaoka, Mika; Koike, Yuko; Yamada, Ryohei; Kubota, Tomohiro; Yoshii, Hideki*; Otani, Kazunori*; Hiyama, Yoshinori*; Kikuchi, Masaaki*; et al.
JAEA-Review 2020-070, 120 Pages, 2021/02
JAEA-Review-2020-070.pdf:2.47MB
Based on the regulations (the safety regulation of Tokai Reprocessing Plant, the safety regulation of nuclear fuel material usage facilities, the radiation safety rule, the regulation about prevention from radiation hazards due to radioisotopes, which are related with the nuclear regulatory acts, the local agreement concerning with safety and environment conservation around nuclear facilities, the water pollution control law, and by law of Ibaraki Prefecture), the effluent control of liquid waste discharged from the Nuclear Fuel Cycle Engineering Laboratories of Japan Atomic Energy Agency has been performed. This report describes the effluent control results of the liquid waste in the fiscal year 2019. In this period, the concentrations and the quantities of the radioactivity in liquid waste discharged from the reprocessing plant, the plutonium fuel fabrication facilities, and the other nuclear fuel material usage facilities were much lower than the limits authorized by the above regulations.
Yamane, Ryo*; Komatsu, Kazuki*; Gochi, Jun*; Uwatoko, Yoshiya*; Machida, Shinichi*; Hattori, Takanori; Ito, Hayate*; Kagi, Hiroyuki*
Nature Communications (Internet), 12, p.1129_1 - 1129_6, 2021/02
Times Cited Count：29 Percentile：84.54(Multidisciplinary Sciences)Ice exhibits extraordinary structural variety in its polymorphic structures. The existence of a new form of diversity in ice polymorphism has recently been debated in both experimental and theoretical studies, questioning whether hydrogen-disordered ice can transform into multiple hydrogen-ordered phases, contrary to the known one-to-one correspondence between disordered ice and its ordered phase. Here we report a new high-pressure phase, ice XIX, which is a second hydrogen-ordered phase of ice VI. This is the first discovery to demonstrate that disordered ice undergoes different manners of hydrogen ordering. Such multiplicity can appear in all disordered ice, and it widely provides a new research approach to deepen our knowledge, for example of the crucial issues of ice: the centrosymmetry of hydrogen-ordered configurations and potentially induced (anti-)ferroelectricity. Ultimately, this research opens up the possibility of completing the phase diagram of ice.
Si
at 14.7 GPa and 800 KMori, Yuichiro*; Kagi, Hiroyuki*; Kakizawa, Sho*; Komatsu, Kazuki*; Shito, Chikara*; Iizuka, Riko*; Aoki, Katsutoshi*; Hattori, Takanori; Sano, Asami; Funakoshi, Kenichi*; et al.
Journal of Mineralogical and Petrological Sciences, 116(6), p.309 - 313, 2021/00
Times Cited Count：0 Percentile：0.02(Mineralogy)The Earth's core is believed to contain some light elements because it is 10% less dense than pure Fe under the corresponding pressure and temperature conditions. Hydrogen, a promising candidate among light elements, has phase relations and physical properties that have been investigated mainly for the Fe-H system. This study specifically examined an Fe-Si-H system using in-situ neutron diffraction experiments to investigate the site occupancy of deuterium of hcp-FezSi hydride at 14.7 GPa and 800 K. Results of Rietveld refinement indicate hcp-FeSi hydride as having deuterium (D) occupancy of 0.24(2) exclusively at the interstitial octahedral site in the hcp lattice. The effect on the site occupancy of D by addition of 2.6 wt% Si into Fe (FeSi) was negligible compared to results obtained from an earlier study of an Fe-D system (Machida et al., 2019).
Komatsu, Yuya*; Shimizu, Ryota*; Wilde, M.*; Kobayashi, Shigeru*; Sasahara, Yuki*; Nishio, Kazunori*; Shigematsu, Kei*; Otomo, Akira*; Fukutani, Katsuyuki; Hitosugi, Taro*
Crystal Growth & Design, 20(9), p.5903 - 5907, 2020/09
Times Cited Count：5 Percentile：53.04(Chemistry, Multidisciplinary)Nakano, Masanao; Fujii, Tomoko; Nagaoka, Mika; Inoue, Kazumi; Koike, Yuko; Yamada, Ryohei; Yoshii, Hideki*; Otani, Kazunori*; Hiyama, Yoshinori*; Kikuchi, Masaaki*; et al.
JAEA-Review 2019-045, 120 Pages, 2020/03
JAEA-Review-2019-045.pdf:2.54MB
Based on the regulations (the safety regulation of Tokai Reprocessing Plant, the safety regulation of nuclear fuel material usage facilities, the radiation safety rule, the regulation about prevention from radiation hazards due to radioisotopes, which are related with the nuclear regulatory acts, the local agreement concerning with safety and environment conservation around nuclear facilities, the water pollution control law, and by law of Ibaraki Prefecture), the effluent control of liquid waste discharged from the Nuclear Fuel Cycle Engineering Laboratories of Japan Atomic Energy Agency has been performed. This report describes the effluent control results of the liquid waste in the fiscal year 2018. In this period, the concentrations and the quantities of the radioactivity in liquid waste discharged from the reprocessing plant, the plutonium fuel fabrication facilities, and the other nuclear fuel material usage facilities were much lower than the limits authorized by the above regulations.
Komatsu, Kazuki*; Klotz, S.*; Machida, Shinichi*; Sano, Asami; Hattori, Takanori; Kagi, Hiroyuki*
Proceedings of the National Academy of Sciences of the United States of America, 117(12), p.6356 - 6361, 2020/03
Times Cited Count：16 Percentile：56.87(Multidisciplinary Sciences)Above 2 GPa the phase diagram of water simplifies considerably and exhibits only two solid phases up to 60 GPa, ice VII and ice VIII. The two phases are related to each other by hydrogen ordering, with the oxygen sub-lattice being essentially the same. Here we present neutron diffraction data to 15 GPa which reveal that the rate of hydrogen-ordering at the ice VII-VIII transition decreases strongly with pressure to reach time scales of minutes at 10 GPa. Surprisingly, the ordering process becomes more rapid again upon further compression. We show that such an unusual change in transition rate can be explained by a slowing-down of the rotational dynamics of water molecules with a simultaneous increase of translational motion of hydrogen under pressure, as previously suspected. The observed crossover in the hydrogen dynamics in ice is likely the origin of various hitherto unexplained anomalies of ice VII in the 10-15 GPa range reported by Raman spectroscopy, X-ray diffraction, and proton conductivity.
without stacking disorder by evacuating hydrogen from hydrogen hydrateKomatsu, Kazuki*; Machida, Shinichi*; Noritake, Fumiya*; Hattori, Takanori; Sano, Asami; Yamane, Ryo*; Yamashita, Keishiro*; Kagi, Hiroyuki*
Nature Communications (Internet), 11, p.464_1 - 464_5, 2020/02
Times Cited Count：45 Percentile：86.98(Multidisciplinary Sciences)Water freezes below 0C at ambient pressure ordinarily to ice I
, with hexagonal stacking sequence. Under certain conditions, ice with a cubic stacking sequence can also be formed, but ideal ice I without stacking-disorder has never been formed until recently. Here we demonstrate a route to obtain ice I without stacking-disorder by degassing hydrogen from the high-pressure form of hydrogen hydrate, C, which has a host framework isostructural with ice I. The stacking-disorder free ice I is formed from C via an intermediate amorphous or nano-crystalline form under decompression, unlike the direct transformations occurring in ice XVI from neon hydrate, or ice XVII from hydrogen hydrate. The obtained ice I shows remarkable thermal stability, until the phase transition to ice I at 250 K, originating from the lack of dislocations. This discovery of ideal ice I will promote understanding of the role of stacking-disorder on the physical properties of ice as a counter end-member of ice I.
