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Journal Articles

Neutron scattering on an aqueous sodium chloride solution in the gigapascal pressure range

Yamaguchi, Toshio*; Yoshida, Koji*; Machida, Shinichi*; Hattori, Takanori

Journal of Molecular Liquids, 365, p.120181_1 - 120181_10, 2022/11

 Times Cited Count:0 Percentile:0.01(Chemistry, Physical)

Neutron scattering measurements were performed on an aqueous 3 mol/kg NaCl solution in D$$_2$$O at temperature and pressure conditions of 0.1 MPa/298K, 1 GPa/298K, 1 GPa/523K, and 4 GPa/523K. The empirical potential structure refinement method was applied to the obtained data to extract the pair correlation function, coordination number distribution, angular distribution (orientation correlation), and spatial density function (3-D structure). From those results, pressure and temperature dependence of solvation and association of ions and solvent-water structure were discussed.

Journal Articles

Hydrogen vibration excitations of ZrH$$_{1.8}$$ and TiH$$_{1.84}$$ 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

 Times Cited Count:0 Percentile:0(Materials Science, Multidisciplinary)

Hydrogen vibration excitations of fluorite-type ZrH$$_{1.8}$$ and TiH$$_{1.84}$$ 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 $$E_1$$(meV) = 141.4(2) + 1.02(2)$$P$$(GPa) and $$E_1$$(meV) = 149.4(1) + 1.21(8)$$P$$(GPa) for ZrH$$_{1.8}$$ and TiH$$_{1.84}$$, respectively. Coupling with pressure dependence of lattice parameters, the relations between metal-hydrogen distance ($$d_{M-H}$$) and $$E_1$$ are found to be well described by the equations $$E_1$$(meV) = 1.62(9)$$times$$ 10$$^3$$ $$d_{M-H}^{-3.31(8)}$$($AA) and $E_1$$(meV) = 1.47(21)$$times$$ 10$$^3$$ $$d_{M-H}^{-3.5(2)}$$(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.

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:0 Percentile:0.03(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:0 Percentile:0(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

Enhancement of electrical conductivity to metallization of Mn$$_{3-x}$$Fe$$_x$$O$$_4$$ spinel and postspinel with elevating pressure

Yamanaka, Takamitsu*; Rahman, S.*; Nakamoto, Yuki*; Hattori, Takanori; Jang, B. G.*; Kim, D. Y.*; Mao, H.-K.*

Journal of Physics and Chemistry of Solids, 167, p.110721_1 - 110721_10, 2022/08

 Times Cited Count:1 Percentile:63.88(Chemistry, Multidisciplinary)

High-pressure neutron diffraction proved that MnFe$$_2$$O$$_4$$ and Mn$$_2$$FeO$$_4$$ spinels transform into CaMn$$_2$$O$$_4$$-type structure above 18 GPa and 14 GPa, respectively. The transition pressure of Mn$$_{3-x}$$Fe$$_x$$O$$_4$$ solutions decreases with increasing Mn content. Synchrotron X-ray M$"{o}$ssbauer experiments revealed that Fe$$^{2+}$$ and Fe$$^{3+}$$ distribution at the tetrahedral (A) and octahedral (B) sites in the spinel structure changes with pressure. MnFe$$_2$$O$$_4$$ and Mn$$_2$$FeO$$_4$$ spinels are ferrimagnetic and the CaMn$$_2$$O$$_4$$-type phase is paramagnetic. The temperature dependence of resistivity indicates that both spinels are semiconductors wherein electrons hop between cations at the A and B sites. A pressure-induced shortening of B-B distance promoted conduction via greater electron mobility between adjacent B cations. The Fe$$^{2+}$$ and Fe$$^{3+}$$ occupancies at the B sites in MnFe$$_2$$O$$_4$$ are much larger than those in Mn$$_2$$FeO$$_4$$. The CaMn$$_2$$O$$_4$$-type phase is metallic. Theoretical calculation confirmed the metallic character and Fe d-orbitals strongly renormalized compared to Mn d-orbitals.

Journal Articles

High-pressure neutron experiments at PLANET in J-PARC using the six-axis multi-anvil press ATSUHIME

Hattori, Takanori

Yukuatsu Gijutsu, 61(7), p.29 - 35, 2022/07

As an example of the application of hydraulic technology, the 6-axis type multi-anvil press "ATSUHIME" in the J-PARC ultra-high pressure neutron diffractometer PLANET and the research on hydrogen in the Earth's core using them are introduced.

Journal Articles

Structure of basaltic glass at pressures up to 18 GPa

Ohashi, Tomonori*; Sakamaki, Tatsuya*; Funakoshi, Kenichi*; Hattori, Takanori; Hisano, Naoki*; Abe, Jun*; Suzuki, Akio*

American Mineralogist, 107(3), p.325 - 335, 2022/03

 Times Cited Count:0 Percentile:0.03(Geochemistry & Geophysics)

The basaltic glass structure were investigated to 18 GPa using in situ X-ray and neutron diffraction. The O-O coordination number (CN$$_textrm{OO}$$) starts to rise with maintaining the mean O-O distance (r$$_textrm{OO}$$) above 2-4 GPa, and then CN$$_textrm{OO}$$ stops increasing and r$$_textrm{OO}$$ begins to shrink along with the increase in the Al-O coordination number (CN$$_textrm{AlO}$$) above 9 GPa. This is interpreted by the change in the contraction mechanism from tetrahedral network bending to oxygen packing ratio increase via the CN$$_textrm{AlO}$$ increase. The oxygen packing fraction exceeds the value for dense random packing, suggesting that the oxygen-packing hypothesis cannot account for the pressure-induced structural transformations of silica and silicate glasses. The CN$$_textrm{OO}$$ increase at 2-4 GPa reflects the elastic softening of silicate glass, which may causes anomalous elastic moduli of basaltic glass at $$sim$$ 2 GPa.

Journal Articles

Structure of an aqueous RbCl solution in the gigapascal pressure range by neutron diffraction combined with empirical potential structure refinement modeling

Zhang, W. Q.*; Yamaguchi, Toshio*; Fang, C. H.*; Yoshida, Koji*; Zhou, Y. Q.*; Zhu, F. Y.*; Machida, Shinichi*; Hattori, Takanori; Li, W.*

Journal of Molecular Liquids, 348, p.118080_1 - 118080_11, 2022/02

 Times Cited Count:1 Percentile:66.16(Chemistry, Physical)

The ion hydration and association and hydrogen-bonded water structure in an aqueous 3 mol/kg RbCl solution were investigated at 298 K/0.1 MPa, 298 K/1 GPa, 523 K/1 GPa, and 523 K/4 GPa by neutron diffraction combined with EPSR methods. The second hydration layer of Rb$$^+$$ and Cl$$^-$$ becomes evident under elevated pressure and temperature conditions. The average oxygen coordination number of Rb$$^+$$ (Cl$$^-$$) in the first hydration layer increases from 6.3 (5.9) ambient pressure to 8.9 (9.1) at 4 GPa, while decreasing coordination distance from 0.290 nm (0.322 nm) to 0.288 nm (0.314 nm). The orientation of the water dipole in the first solvation shell of Rb$$^+$$ and a central water molecule is sensitive to pressure, but that in the first solvation shell of Cl$$^-$$ does not change very much. The number of contact-ion pairs Rb$$^+$$-Cl$$^-$$ decreases with elevated temperature and increases with elevated pressure. Water molecules are closely packed, and the tetrahedral hydrogen-bonded network of water molecules no longer exists in extreme conditions.

Journal Articles

Development of a hybrid piston cylinder cell for quasielastic neutron scattering experiments up to 1 GPa

Hattori, Takanori; Kawamura, Seiko; Kawasaki, Takuro

High Pressure Research, 42(2), p.226 - 235, 2022/00

 Times Cited Count:0 Percentile:0(Physics, Multidisciplinary)

We have developed a hybrid piston cylinder cell for quasi-elastic neutron scattering (QENS) experiments up to about 1 GPa. It consists of a fretted cylinder made of the high tensile steel (SNCM439) liner and the Al alloy (NA700) jacket. Performance tests revealed that the cell can withstand a pressure of 0.8 GPa without irreversible damage and has 4.4 times larger neutron transmission at 3.14 meV (5.10${AA}$ in wavelength) than that of a conventional CuBe monobloc cylinder. Combined with the sample assembly devised for suppressing multiple scattering, high quality QENS spectra of water were obtained up to 0.8 GPa. This study illustrates the efficacy of the hybrid cylinders not only for increasing maximum available pressure but also manipulating the available pressure and the signal intensity, depending on the purpose of the experiments.

Journal Articles

Crystalline fully carboxylated polyacetylene obtained under high pressure as a Li-ion battery anode material

Wang, X.*; Tang, X.*; Zhang, P.*; Wang, Y.*; Gao, D.*; Liu, J.*; Hui, K.*; Wang, Y.*; Dong, X.*; Hattori, Takanori; et al.

Journal of Physical Chemistry Letters (Internet), 12(50), p.12055 - 12061, 2021/12

 Times Cited Count:3 Percentile:38.89(Chemistry, Physical)

Substituted polyacetylene is expected to improve the chemical stability, physical properties, and additional functions of the polyacetylene backbones, but its diversity is very limited. Here, by applying external pressure on solid acetylenedicarboxylic acid, we report the first crystalline poly-dicarboxylacetylene with every carbon on the trans-polyacetylene backbone bonded to a carboxyl group, which is very hard to synthesize by traditional methods. This unique structure combines the extremely high content of carbonyl groups and high conductivity of a polyacetylene backbone, which exhibits a high specific capacity and excellent cycling/rate performance as a Li-ion battery (LIB) anode. We present a completely functionalized crystalline polyacetylene and provide a high-pressure solution for the synthesis of polymeric LIB materials and other polymeric materials with a high content of active groups.

Journal Articles

Synthesis and characterisation of a new graphitic C-S compound obtained by high pressure decomposition of CS$$_2$$

Klotz, S.*; Baptiste, B.*; Hattori, Takanori; Feng, S. M.*; Jin, Ch.*; B$'e$neut, K.*; Guigner, J. M.*; Est$`e$ve, I.*

Carbon, 185, p.491 - 500, 2021/11

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

Carbon disulphide (CS$$_2$$) is one of the simplest molecular systems made of double covalent bonds. Under high pressure, the molecular structure is expected to break up to form extended crystalline or polymeric solids. Here we show that by compression at 300 K to approximately $$sim$$10 GPa using large-volume high pressure techniques, an instantaneous reaction leads to a mixture of pure sulphur and a well-defined compound with stoichiometry close to C$$_2$$S which can be recovered to ambient pressure. We present neutron and X-ray diffraction as well as Raman data which show that this material consists of sulphur bonded to sp$$^2$$ graphite layers of nanometric dimensions. The compound is a semiconductor with a gap of 45 meV, as revealed by temperature dependent resistivity measurements, and annealing at temperatures above 200$$^{circ}$$C allow to reduce its sulphur content up to C$$_{10}$$S. Its structural and electronic properties are fundamentally different to "Bridgman black" reported from previous high pressure experiments on CS$$_2$$.

Journal Articles

Phase transition and chemical reactivity of 1H-tetrazole under high pressure up to 100 GPa

Gao, D.*; Tang, X.*; Wang, X.*; Yang, X.*; Zhang, P.*; Che, G.*; Han, J.*; Hattori, Takanori; Wang, Y.*; Dong, X.*; et al.

Physical Chemistry Chemical Physics, 23(35), p.19503 - 19510, 2021/09

 Times Cited Count:4 Percentile:53.88(Chemistry, Physical)

Pressure-induced phase transition and polymerization of nitrogen-rich molecules are widely focused due to its extreme importance for the development of green high energy density materials. Here, we present a study of the phase transition and chemical reaction of 1H-tetrazole up to 100 GPa by using ${it in situ}$ Raman, IR, X-ray diffraction, neutron diffraction techniques and theoretical calculation. A phase transition above 2.6 GPa was identified and the high-pressure structure was determined with one molecule in a unit cell. The 1H-tetrazole polymerizes reversibly below 100 GPa, probably through a carbon-nitrogen bonding instead of nitrogen-nitrogen bonding. Our studies updated the structure model of the high pressure phase of 1H-tetrazole, and presented the possible intermolecular bonding route for the first time, which gives new insights to understand the phase transition and chemical reaction of nitrogen-rich compounds, and benefit for designing new high energy density materials.

Journal Articles

Behavior of light elements in iron-silicate-water-sulfur system during early Earth's evolution

Iizuka, Riko*; Goto, Hirotada*; Shito, Chikara*; Fukuyama, Ko*; Mori, Yuichiro*; Hattori, Takanori; Sano, Asami; Funakoshi, Kenichi*; Kagi, Hiroyuki*

Scientific Reports (Internet), 11(1), p.12632_1 - 12632_10, 2021/06

 Times Cited Count:2 Percentile:26.42(Multidisciplinary Sciences)

The Earth's core consist of Fe-Ni alloy with some light elements (H, C, O, Si, S etc.). Hydrogen (H) is the most abundant element in the universe and one of the promising candidates. In this study, we have investigated the effects of sulfur(S) on hydrogenation of iron-hydrous silicate system containing saturated water in the ideal composition of the primitive Earth. We observed a series of phase transitions of Fe, dehydration of the hydrous mineral, and formation of olivine and enstatite with increasing temperature. The FeS formed as the coexisting phase of Fe under high-pressure and temperature condition, but its unit cell volume did not increase, suggesting that FeS is hardly hydrogenated. Recovered samples exhibited that H and S can be incorporated into solid Fe, which lowers the melting temperature as Fe(H$$_{x}$$)-FeS system. No detection of other light elements (C, O, Si) in solid Fe suggests that they dissolve into molten iron hydride and/or FeS in the later process of Earth's core-mantle differentiation.

Journal Articles

Crystal structure of nesquehonite, MgCO$$_{3}$$ $$cdot$$ 3H(D)$$_{2}$$O by neutron diffraction and effect of pH on structural formulas of nesquehonite

Yamamoto, Genichiro*; Kyono, Atsushi*; Abe, Jun*; Sano, Asami; Hattori, Takanori

Journal of Mineralogical and Petrological Sciences, 116(2), p.96 - 103, 2021/04

 Times Cited Count:2 Percentile:46.2(Mineralogy)

Neutron diffraction, Raman spectroscopy, and thermal analysis were performed to investigate the composition, structure, and formation conditions of the magnesium carbonate hydrate nesquehonite. The time-of-flight neutron diffraction revealed the crystal structure of the monoclinic space group $$P$$2$$_{1}/n$$ with lattice parameters of $$a$$=7.72100(12)$AA, $b$$=5.37518(7)$AA, $c$$=12.1430(3)$AA, $beta$$=90.165(4)$$^circ$$, in which two deuterium atoms are coordinated to the O1, O2, and O6 atoms to form water molecules. The three water molecules in the structure suggests the structural formula of the nesquehonite should be MgCO$$_{3}$$ $$cdot$$ 3H$$_{2}$$O rather than Mg(HCO$$_{3}$$)(OH) $$cdot $$2H$$_{2}$$O.

Journal Articles

High-pressure and high-temperature neutron-diffraction experiments using Kawai-type multi-anvil assemblies

Sano, Asami; Kakizawa, Sho*; Shito, Chikara*; Hattori, Takanori; Machida, Shinichi*; Abe, Jun*; Funakoshi, Kenichi*; Kagi, Hiroyuki*

High Pressure Research, 41(1), p.65 - 74, 2021/03

 Times Cited Count:2 Percentile:49.19(Physics, Multidisciplinary)

We applied Kawai-type multi-anvil assemblies (MA6-8) for time-of-flight neutron-diffraction experiments to achieve high pressures and high temperatures simultaneously. To achieve sufficient signal intensities, the angular access to the sample was enlarged using slits and tapers on the first-stage anvils. Using SiC-binder sintered diamond for the second-stage anvils that transmits neutrons, sufficient signal intensities were achieved at a high-pressure of $$sim$$23.1 GPa. A high-temperature experiment was also conducted at 16.2 GPa and 973 K, validating the use of tungsten carbide for the second-stage anvils. The present study reveals the capability of the MA6-8 cells in neutron-diffraction experiments to attain pressures and temperatures beyond the limits of the conventional MA6-6 cells used in the high-pressure neutron diffractometer PLANET at the MLF, J-PARC.

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:5 Percentile:78.39(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

Pressure-dependent structure of methanol-water mixtures up to 1.2 GPa; Neutron diffraction experiments and molecular dynamics simulations

Temleitner, L.*; Hattori, Takanori; Abe, Jun*; Nakajima, Yoichi*; Pusztai, L.*

Molecules (Internet), 26(5), p.1218_1 - 1218_12, 2021/03

 Times Cited Count:0 Percentile:0(Biochemistry & Molecular Biology)

Total structure factors of per-deuterated methanol and heavy water, CD$$_{3}$$OD and D$$_{2}$$O, have been determined across the entire composition range at pressures of up to 1.2 GPa, by neutron diffraction. Largest variations due to increasing pressure were observed below $$Q=$$ 5 $AA$^{-1}$$, mostly as shifts of the first and second maxima. Molecular dynamics computer simulations been conducted at the experimental pressures to interpret neutron diffraction results. The peak shifts mentioned above could be qualitatively reproduced by simulations. In order to reveal the influence of changing pressure on the local intermolecular structure, simulated structures have been analyzed in terms of hydrogen bond related partial radial distribution functions and size distributions of hydrogen bonded cyclic entities. Distinct differences between pressure dependent structures of water-rich and methanol-rich composition regions have been revealed.

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:0 Percentile:0(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

Suppressed lattice disorder for large emission enhancement and structural robustness in hybrid lead iodide perovskite discovered by high-pressure isotope effect

Kong, L.*; Gong, J.*; Hu, Q.*; Capitani, F.*; Celeste, A.*; Hattori, Takanori; Sano, Asami; Li, N.*; Yang, W.*; Liu, G.*; et al.

Advanced Functional Materials, 31(9), p.2009131_1 - 2009131_12, 2021/02

 Times Cited Count:14 Percentile:79.39(Chemistry, Multidisciplinary)

The soft nature of organic-inorganic halide perovskites renders their lattice particularly tunable to external stimuli such as pressure, undoubtedly offering an effective way to modify their structure for extraordinary optoelectronic properties. However, these soft materials meanwhile feature a general characteristic that even a very mild pressure will lead to detrimental lattice distortion and weaken the critical light-matter interaction, thereby triggering the performance degradation. Here, using the methylammonium lead iodide as a representative exploratory platform, we observed the pressure-driven lattice disorder can be significantly suppressed via hydrogen isotope effect, which is crucial for better optical and mechanical properties previously unattainable.

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:16 Percentile:88.6(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.

278 (Records 1-20 displayed on this page)