High-precision powder diffraction experiments under high pressure at the J-PARC PLANET beamline and recent results; Observation of hydrogen bond symmetrization in ice

Hattori, Takanori; Komatsu, Kazuki*

Nihon Genshiryoku Gakkai-Shi ATOMO, 66(12), p.618 - 622, 2024/12

https://doi.org/10.3327/jaesjb.66.12_618

The high-pressure neutron diffractometer PLANET is the first beamline dedicated to high-pressure neutron experiments in Japan. It was constructed at the Materials and Life Science Experimental Facility (MLF) in the Japan Proton Accelerator Research Complex (J-PARC) located at Tokai-mura in Ibaraki Prefecture. Energy-dispersive data measurement using pulsed neutrons, state-of-the-art optical instruments, and a high-pressure device enable us to analyze the structure of crystals, liquids, and glasses over a wide range of pressure and temperature with unprecedented accuracy. In this paper, we will show how this has been achieved and introduce the recently published results on the symmetrization of hydrogen bonds in ice.

Hydrogen bond symmetrisation in DO 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

https://doi.org/10.1038/s41467-024-48932-8

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 DO 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.

Single-crystal structure analysis of non-deuterated triglycine sulfate by neutron diffraction at 20 and 298 K; A New disorder model for the 298 K structure

Terasawa, Yukana*; Ohara, Takashi; Sato, Sota*; Yoshida, Satoshi*; Asahi, Toru*

Acta Crystallographica Section E; Crystallographic Communications (Internet), 78(3), p.306 - 312, 2022/03

https://doi.org/10.1107/S2056989022000858

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.

Ab initio path integral molecular dynamics simulation study on the dihydrogen bond of NH BeH

Hayashi, Aiko*; Shiga, Motoyuki; Tachikawa, Masanori*

Chemical Physics Letters, 410(1-3), p.54 - 58, 2005/07

https://doi.org/10.1016/j.cplett.2005.05.035

Hydrogen bond is conventionally a bonding between hydrogen and an atom with high electronegativity such as fluorine, oxygen or nitrogen. A dihydrogen bond is an exceptional case, which is an attractive force between positively and negatively charged hydrogen atoms. In this report, some characters of the dihydrogen bond is studied in detail for the molecular cluster BeHNH using ab initio molecular dynamics simulation.

High resolution neutron protein crystallography, hydrogen and hydration in proteins

Niimura, Nobuo; Chatake, Toshiyuki; Ostermann, A.; Kurihara, Kazuo; Tanaka, Ichiro

Zeitschrift fr Kristallographie, 218(2), p.96 - 107, 2003/03

no abstracts in English

Study of vibrational spectra of interlayer water in Na-Smectite by means of molecular dynamics simulations

Suzuki, Satoru; Kawamura, Katsuyuki*

JNC TN8400 2001-005, 41 Pages, 2001/04

JNC-TN8400-2001-005.pdf:1.1MB

A correlation between molecular structure and a vibrational spectrum of interlayer water in Na-smectite was investigated by means of Molecular Dymamics (MDs) simulations. Detailed comparison of simulation results with IR spectroscopic observations for the water-smectite system indicated good agreement. Internal vibrational spectra of water were obtained by the Fourier transformation of velocty auto-correlation function of hydrogen atom. A stretching vibrational spectrum of interlayer water consisted of a broad band with a peak top around 3400cm and a sharp peak around 3650 to 3700cm. The fomer broad band was assigned to O-H vibrations between water molecules as bulk water, while the latter band was attributed to O-H ones oriented to siloxane surface through hydrogen bonding. The hydrogen bond distance, determined as the shortest O-O distance by the radial distribution function (RDF), revealed that hydrogen bond distance between water and siloxane surface (O-O 3.0 -O = ca. 2.8 AA ). These results suggested that interaction between water molecule and siloxane surface weaker than that between water molecules, although they were forced to be oriented.

Effect of hydrogen bonding on laser-induced transfer of 1-pyrenebutyric acid in solid polymers

Saito, Kenichi*; Ichinose, Yuji; Kawanishi, Shunichi; Fukumura, H.*

Chemical Physics Letters, 291(3-4), p.433 - 437, 1998/00

https://doi.org/10.1016/S0009-2614(98)00579-X

no abstracts in English

Pressure induced hydrogen bond symmetrization in a hydrous mineral

Sano, Asami; Hattori, Takanori; Komatsu, Kazuki*; Kagi, Hiroyuki*; Nagai, Takaya*

no journal, , 

Hydrogen exists not only on the Earth's surface as liquid water but also incorporated into minerals in the deep mantle as hydroxyl ion. At ambient pressure on the surface of the Earth, hydrogen in minerals generally takes an asymmetric position between two oxygen atoms, which forms a short covalent bond on the one side and a long and relatively weak hydrogen bond on the other side. However, it was theoretically predicted in 1970' that the hydrogen in ice locates at the center between two oxygen atoms under high pressure, which is so-called symmetrization of hydrogen bond. To investigate how the symmetrization affects on the physical properties of minerals, we conducted neutron diffraction experiments on -AlOOH at high pressure. We observed that hydrogen reaches at the center between two oxygen atoms at 18.1 GPa. The present study revealed that even small change of hydrogen atomic position but the symmetrization can change the physical property of mineral.