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Journal Articles

Crystal structure and compressibility of magnesium chloride heptahydrate found under high pressure

Yamashita, Keishiro*; Komatsu, Kazuki*; Hattori, Takanori; Machida, Shinichi*; Kagi, Hiroyuki*

Acta Crystallographica Section B; Structural Science, Crystal Engineering and Materials (Internet), 80(6), p.695 - 705, 2024/12

So far, the odd hydration number has been missing in the water-rich magnesium chloride hydrate series (MgCl$$_2$$$$cdot$$$$n$$H$$_2$$O). In this study, we have identified magnesium chloride heptahydrate, MgCl$$_2$$$$cdot$$7H$$_2$$O (or MgCl$$_2$$$$cdot$$7D$$_2$$O) which forms at high pressures and high temperatures of above 2 GPa and above 300 K, respectively. Its structure has been determined by a combination of ${it in-situ}$ single crystal X-ray diffraction at 2.5 GPa and 298 K and powder neutron diffraction at 3.1 GPa and 300 K. The results showed an orientational disorder of water molecules, which was also examined by the density-functional-theory calculations. The disorder involves the reconnection of hydrogen bonds, which differs from those in water ice phases and known disordered salt hydrates. The shrinkage by compression occurs mainly in one direction. In the plane perpendicular to this most compressible direction, oxygen and chlorine atoms are in a hexagonal-like arrangement.

Journal Articles

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

 Times Cited Count:0 Percentile:0.00(Chemistry, Physical)

High-pressure responses of the O-D$$cdotcdotcdot$$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)$$_{0.920(12)}$$F$$_{1.080(12)}$$ 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$$^{-1}$$. 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$$^{-1}$$ 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.

Journal Articles

Hydrogen bond symmetrisation in D$$_2$$O 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

 Times Cited Count:0 Percentile:0.00(Multidisciplinary Sciences)

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 D$$_2$$O 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.

Journal Articles

Securing reversibility of U$$^{V}$$O$$_{2}$$$$^{+}$$/U$$^{VI}$$O$$_{2}$$$$^{2+}$$redox equilibrium in [emim]Tf$$_{2}$$N-based liquid electrolytes towards uranium redox-flow battery

Takao, Koichiro*; Ouchi, Kazuki; Komatsu, Atsushi; Kitatsuji, Yoshihiro; Watanabe, Masayuki

European Journal of Inorganic Chemistry, 27(14), p.e202300787_1 - e202300787_7, 2024/05

 Times Cited Count:0 Percentile:0.00(Chemistry, Inorganic & Nuclear)

Electrochemical behavior of U$$^{rm V}$$O$$_{2}$$$$^{+}$$/U$$^{rm VI}$$O$$_{2}$$$$^{2+}$$ in 1-ethyl-3-methylimidazolium bis(trifluoromethyl)sulfonylamide ([emim]Tf$$_{2}$$N) ionic liquid was studied to clarify what are required to attain its redox reversibility for utilizing depleted U as an electrode active material in a redox flow battery. As a result, reversibility of the U$$^{rm V}$$O$$_{2}$$$$^{+}$$/U$$^{rm VI}$$O$$_{2}$$$$^{2+}$$ redox reaction was successfully achieved in use of a glassy carbon working electrode under presence of Cl$$^{-}$$ in [emim]Tf$$_{2}$$N. To improve diffusivity of solutes, [emim]Tf$$_{2}$$N diluted with an auxiliary molecular solvent, N,N-dimethylformamide (DMF). We have succeeded in demonstrating a reversible redox reaction of [U$$^{rm VI}$$O$$_{2}$$Cl$$^{4}$$]$$^{2-}$$ + e$$^{-}$$ = [U$$^{rm V}$$O$$_{2}$$Cl$$^{4}$$]$$^{3-}$$ in the 50:50 v/v [emim]Tf$$_{2}$$N-DMF liquid electrolyte containing Cl$$^{-}$$.

Journal Articles

Slightly hydrogen-ordered state of ice IV evidenced by ${it in situ}$ neutron diffraction

Kobayashi, 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:2 Percentile:23.97(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 ${it in situ}$ powder neutron diffraction experiments for DCl-doped D$$_{2}$$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.

Journal Articles

The Hydrogen-bond network in sodium chloride tridecahydrate; Analogy with ice VI

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:1 Percentile:37.25(Chemistry, Multidisciplinary)

The structure of a recently-found hyperhydrated form of sodium chloride, NaCl$$cdot$$ 13H(D)$$_{2}$$O, has been determined by ${it in situ}$ 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.

Journal Articles

Hydrogen occupation and hydrogen-induced volume expansion in Fe$$_{0.9}$$Ni$$_{0.1}$$D$$_x$$ at high $$P-T$$ conditions

Shito, 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:3 Percentile:71.64(Geochemistry & Geophysics)

The phase relation and crystal structure of Fe$$_{0.9}$$Ni$$_{0.1}$$H$$_x$$ (D$$_x$$) at high pressures and temperatures up to 12 GPa and 1000 K were clarified by in-situ X-ray and neutron diffraction measurements. Under $$P-T$$ conditions of the present study, no deuterium atoms occupied tetragonal ($$T$$) sites of face-centered cubic (fcc) Fe$$_{0.9}$$Ni$$_{0.1}$$D$$_x$$ unlike fcc FeH$$_x$$(D$$_x$$). The deuterium-induced volume expansion per deuterium $$v_mathrm{D}$$ was determined as 2.45(4) $AA$^3$$ and 3.31(6) $AA$^3$$ for fcc and hcp phases, respectively, which were significantly larger than the corresponding values for FeD$$_x$$. The $$v_mathrm{D}$$ 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 $$v_mathrm{D}$$ 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.

Journal Articles

Magnetic and structure transition of Mn$$_{3-x}$$Fe$$_x$$O$$_4$$ solid solutions under high-pressure and high-temperature conditions

Yamanaka, 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:1 Percentile:11.61(Materials Science, Multidisciplinary)

Magnetic and crystal structure of Mn$$_{3-x}$$Fe$$_x$$O$$_4$$ solid solutions under high-PT conditions are investigated by neutron diffraction and synchrotron M${"o}$ssbauer spectroscopy. The ferrimagnetic-paramagnetic transition and tetragonal-cubic transition of Mn$$_2$$FeO$$_4$$ spinel occur at 100$$^circ$$C and 180$$^circ$$C, respectively, suggesting both the transitions are not coupled. The structure transition temperature decreases with pressure. M${"o}$ssbauer experiments and neutron diffraction revealed that the Fe$$^{2+}$$ occupancy in tetrahedral site increases increase with pressure, suggesting Mn$$_2$$FeO$$_4$$ phase approaches inverse spinel. Magnetic structure refinement clarified paramagnetic and ferrimagnetic structure of MnFe$$_2$$O$$_4$$ and Mn$$_2$$FeO$$_4$$. These spinels transform into high-pressure orthorhombic phases at 18.4 and 14.0 GPa, respectively, indicating lower transition pressure with increasing Mn content.

Journal Articles

Atomic distribution and local structure in ice VII from in situ neutron diffraction

Yamashita, Keishiro*; Komatsu, Kazuki*; Klotz, S.*; Fabelo, O.*; Fern$'a$ndez-D$'i$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:3 Percentile:20.85(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.

Journal Articles

Improvement of nano-polycrystalline diamond anvil cells with Zr-based bulk metallic glass cylinder for higher pressures; Application to Laue-TOF diffractometer

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:46.06(Physics, Multidisciplinary)

Journal Articles

Electrochemical studies of uranium (IV) in an ionic liquid-DMF mixture to build a redox flow battery using uranium as an electrode active material

Ouchi, Kazuki; Komatsu, Atsushi; Takao, Koichiro*; Kitatsuji, Yoshihiro; Watanabe, Masayuki

Chemistry Letters, 50(6), p.1169 - 1172, 2021/06

 Times Cited Count:2 Percentile:11.15(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$$^{III}$$/U$$^{IV}$$ couple that could be applied to the anode reaction of the RFB.

Journal Articles

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

 Times Cited Count:11 Percentile:73.68(Chemistry, Inorganic & Nuclear)

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 ${AA}$). 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 ${AA}$ again, implying the pressure-induced reformation of the dihydrogen bonds. Furthermore, the HP1 transformed to the second one with the structure of $$P2_1$$ (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 ${AA}$. The present study experimentally first confirmed the breakage and reformation of the dihydrogen bonds by the structural change under pressure.

Journal Articles

Origin of magnetovolume effect in a cobaltite

Miao, P.*; Tan, Z.*; Lee, S. H.*; Ishikawa, Yoshihisa*; Torii, Shuki*; Yonemura, Masao*; Koda, Akihiro*; Komatsu, Kazuki*; Machida, Shinichi*; Sano, Asami; et al.

Physical Review B, 103(9), p.094302_1 - 094302_18, 2021/03

 Times Cited Count:3 Percentile:21.40(Materials Science, Multidisciplinary)

The layered perovskite PrBaCo$$_{2}$$O$$_{5.5}$$ demonstrates a strong negative thermal expansion (NTE) which holds potential for being fabricated into composites with zero thermal expansion. The NTE was found to be intimately associated with the spontaneous magnetic ordering, known as magneto-volume effect (MVE). Here we report with compelling evidences that the continuous-like MVE in PrBaCo$$_{2}$$O$$_{5.5}$$ is intrinsically of discontinuous character, originating from an magnetoelectric transition from an antiferromagnetic insulating large-volume (AFILV) phase to a ferromagnetic less-insulating small-volume (FLISV) phase. Furthermore, the magnetoelectric effect (ME) shows high sensitivity to multiple external stimuli such as temperature, carrier doping, hydrostatic pressure, magnetic field etc. In contrast to the well-known ME such as colossal magnetoresistance and multi-ferroic effect which involve symmetry breaking of crystal structure, the ME in the cobaltite is purely isostructural. Our discovery provides a new path way to realizing the ME as well as the NTE, which may find applications in new techniques.

Journal Articles

Morphological reproductive characteristics of testes and fertilization capacity of cryopreserved sperm after the Fukushima accident in raccoon (${it Procyon lotor}$)

Komatsu, Kazuki*; Iwasaki, Tsugumi*; Murata, Kosuke*; Yamashiro, Hideaki*; Goh, V. S. T.*; Nakayama, Ryo*; Fujishima, Yohei*; Ono, Takumi*; Kino, Yasushi*; Shimizu, Yoshinaka*; et al.

Reproduction in Domestic Animals, 56(3), p.484 - 497, 2021/03

 Times Cited Count:10 Percentile:83.43(Agriculture, Dairy & Animal Science)

We have established an archive system of livestock and wild animals from the surrounding ex-evacuation zone. Wildlife within the alert zone have been exposed to low-dose-rate (LDR) radiation for a long and continuous time. In this study, we analysed the morphological characteristics of the testes and in vitro fertilization (IVF) capacity of cryopreserved sperm of raccoons from the ex-evacuation zone of the FDNPP accident. This study revealed that the chronic and LDR radiation exposure associated with the FDNPP accident had no adverse effect on the reproductive characteristics and functions of male raccoons.

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:36 Percentile:84.45(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

Neutron diffraction study of hydrogen site occupancy in Fe$$_{0.95}$$Si$$_{0.05}$$ at 14.7 GPa and 800 K

Mori, 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:2 Percentile:13.89(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-Fez$$_{0.95}$$Si$$_{0.05}$$ hydride at 14.7 GPa and 800 K. Results of Rietveld refinement indicate hcp-Fe$$_{0.95}$$Si$$_{0.05}$$ 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 (Fe$$_{0.95}$$Si$$_{0.05}$$) was negligible compared to results obtained from an earlier study of an Fe-D system (Machida et al., 2019).

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:7 Percentile:89.27(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, et.al., 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:20 Percentile:60.20(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

Developments of nano-polycrystalline diamond anvil cells for neutron diffraction experiments

Komatsu, Kazuki*; Klotz, S.*; Nakano, Satoshi*; Machida, Shinichi*; Hattori, Takanori; Sano, Asami; Yamashita, Keishiro*; Irifune, Tetsuo*

High Pressure Research, 40(1), p.184 - 193, 2020/02

 Times Cited Count:14 Percentile:70.11(Physics, Multidisciplinary)

A new high pressure cells for neutron diffraction experiments using nano-polycrystalline anvil is presented. The cell design, off-line pressure generation tests and a gas-loading procedure for this cell are described. The performance is illustrated by powder neutron diffraction patterns of ice VII to $$sim$$ 82 GPa. We also demonstrate the feasibility of single crystal neutron diffraction experiments of Fe$$_{3}$$O$$_{4}$$ at ambient conditions using this cell and discuss the current limitation and future developments.

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, p.464_1 - 464_5, 2020/02

 Times Cited Count:56 Percentile:87.92(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$$_{rm h}$$.

107 (Records 1-20 displayed on this page)