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Journal Articles

Experimental evidence for the existence of a second partially-ordered phase of ice VI

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:1 Percentile:14.36(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.

Journal Articles

Slow compression of crystalline ice at low temperature

Bauer, R.*; Tse, J. S.*; Komatsu, Kazuki*; Machida, Shinichi*; Hattori, Takanori

Nature, 585(7825), p.E9 - E10, 2020/09

 Times Cited Count:0 Percentile:100(Multidisciplinary Sciences)

Pressure-induced structural transformations in deuterated crystalline ice-Ih were studied in-situ at 100 K using neutron diffraction. Very long relaxation time was allowed between small pressure increments to promote transformations to the thermodynamic stable high pressure crystalline phases. The results contradict a recent report in which measurements under similar temperature and pressure environment show successive crystal-to-crystal transformations (Tulk,, Nature 2019). Instead, ice Ih was found to transform partially to an amorphous form (high density amorphous, HDA) at 1.0 GPa and then ice VII started to emerge at 1.5 GPa, a pressure substantially lower than all earlier studies. During this pressure interval, crystalline ice Ih or ice VII co-exist with HDA. The ice VII formed is stable upon pressure release down to 0.1 GPa. The very low compression rate has a profound effect on the crystallinity in the amorphous regime. Gathering all the existing experimental evidences allows an unambiguous description of the phenomenon of pressure induced amorphization. The onset of the phase transition is triggered by a shear instability of the ice lattice. The co-existence ice VII with HDA, instead of the equilibrium thermodynamic stable and proton-ordered ice-VIII under the same pressure-temperature condition reveals at low temperature there is insufficient thermal energy to overcome the substantial geometrical rearrangement from a single proton disordered H-bond network to an interpenetrating proton ordered H-bond crystalline network. Thus, leaving the proton disordered H-network intact. The analysis shows unequivocally that the structure obtained from the compression of ice is controlled by kinetics and dependent on the temperature.

Journal Articles

Anomalous hydrogen dynamics of the ice VII-VIII transition revealed by high-pressure neutron diffraction

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:2 Percentile:64.45(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.

Journal Articles

Ice I$$_{rm c}$$ without stacking disorder by evacuating hydrogen from hydrogen hydrate

Komatsu, Kazuki*; Machida, Shinichi*; Noritake, Fumiya*; Hattori, Takanori; Sano, Asami; Yamane, Ryo*; Yamashita, Keishiro*; Kagi, Hiroyuki*

Nature Communications (Internet), 11(1), p.464_1 - 464_5, 2020/02

 Times Cited Count:6 Percentile:13.29(Multidisciplinary Sciences)

Water freezes below 0$$^{circ}$$C at ambient pressure ordinarily to ice I$$_{rm h}$$, with hexagonal stacking sequence. Under certain conditions, ice with a cubic stacking sequence can also be formed, but ideal ice I$$_{rm c}$$ without stacking-disorder has never been formed until recently. Here we demonstrate a route to obtain ice I$$_{rm c}$$ without stacking-disorder by degassing hydrogen from the high-pressure form of hydrogen hydrate, C$$_{2}$$, which has a host framework isostructural with ice I$$_{rm c}$$. The stacking-disorder free ice I$$_{rm c}$$ is formed from C$$_{2}$$ 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$$_{rm c}$$ shows remarkable thermal stability, until the phase transition to ice I$$_{rm h}$$ at 250 K, originating from the lack of dislocations. This discovery of ideal ice I$$_{rm c}$$ will promote understanding of the role of stacking-disorder on the physical properties of ice as a counter end-member of ice I$$_{rm h}$$.

Journal Articles

Thin ice target for $$^{16}$$O (p,p') experiment

Kawabata, Takahiro*; Akimune, Hidetoshi*; Fujimura, Hisako*; Fujita, Hirohiko*; Fujita, Yoshitaka*; Fujiwara, Mamoru; Hara, Keigo*; Hatanaka, Kichiji*; Hosono, K.*; Ishikawa, Takatsugu*; et al.

Nuclear Instruments and Methods in Physics Research A, 459(1-2), p.171 - 176, 2001/02

 Times Cited Count:17 Percentile:22.98(Instruments & Instrumentation)

no abstracts in English

JAEA Reports

Pu(IV) Nitrate crystallization behavior confirmation experiment

*; *; *; *

JNC-TJ8400 2000-061, 92 Pages, 2000/03


Crystallization procedure is considered to have an advantage in recovering rather pure uranium from contaminated uranium solution and to be applicable for a new reprocessing process. It was confirmed until last year that the reprocessing process with crystallization procedure has a sufficient advantage. But the data for Pu crystallization is very rare. although it is necessary for design of the process with crystallization procedure. In this study, a beaker scale plutonium test was performed in AEA Technology Harwell Laboratory to confirm a behavior of Pu (IV) nitrate under crystallization condition. The results were examined by Mitsubishi Materials Corporation. Test item was a measurement of temperature in case of Pu (IV) nitrate crystallization or freezing of the solution in the following six parameters. (Pu(g/L):200, 100, 50, HNO$$_{3}$$(m):6, Pu valence:4). (Pu(g/L):200, 100, 50, HNO$$_{3}$$(m):4, Pu valence:4). Test results were as follows. (1)Pu(IV) nitrate crystallization was not observed even in the case 200g Pu/L and HNO$$_{3}$$ 6M and 4M which were considered to the best condition but crystal of H$$_{2}$$O and HNO$$_{3}$$ $$cdot$$ 3H$$_{2}$$O were observed. (2)Similar results were obtained for the other parameter with lower Pu concentration. (3)We can estimate that Pu(IV) nitrate crystallization will not occurred in the reprocessing process with crystallization procedure. (4)The solubility data of Pu(NO$$_{3}$$)$$_{4}$$ - HNO$$_{3}$$-H$$_{2}$$O system was obtained.

JAEA Reports

Engineering design of advanced marine reactor MRX

JAERI-Tech 97-045, 601 Pages, 1997/10


no abstracts in English

Journal Articles

Oral presentation

Altitudinal distribution of the Last Interglacial Marine Formation in the central Kanto Plain, Japan

Miyamoto, Tatsuki*; Sugai, Toshihiko*; Komatsu, Tetsuya; Nakanishi, Toshimichi*; Niwa, Yuichi*; Hiura, Yuki

no journal, , 

no abstracts in English

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