An X-ray and neutron scattering study of aqueous MgCl solution in the gigapascal pressure range

Yamaguchi, Toshio*; Fukuyama, Nami*; Yoshida, Koji*; Katayama, Yoshinori*; Machida, Shinichi*; Hattori, Takanori

Liquids, 3(3), p.288 - 302, 2023/09

https://doi.org/10.3390/liquids3030019

We report the structure of an aqueous 2 mol/kg MgCl solution at pressures from 0.1 MPa to 4 GPa and temperatures from 300 to 500 K revealed by X-ray and neutron scattering measurements. The scattering data are analyzed by empirical potential structure refinement (EPSR) modeling to derive the pair distribution functions, coordination number distributions, angle distributions, and spatial density functions as a function of pressure and temperature. Mg forms rigid solvation shells extended to the third shell; the first solvation shell of six-fold octahedral coordination with about six water molecules at 0 GPa transforms into about five water molecules and one Cl due to the formation of the contact ion pairs in the GPa pressure range. The Cl solvation shows a substantial pressure dependence; the coordination number of a water oxygen atom around Cl increases from 8 at 0.1 MPa/300 K to 10 at 4 GPa/500 K. The solvent water transforms the tetrahedral network structure at 0.1 MPa/300 K to a densely packed structure in the GPa pressure range; the number of water oxygen atoms around a central water molecule gradually increases from 4.6 at 0.1 MPa/298 K to 8.4 at 4 GPa/500 K.

Level structures of Ca cast doubt on a doubly magic Ca

Chen, S.*; Browne, F.*; Doornenbal, P.*; Lee, J.*; Obertelli, A.*; Tsunoda, Yusuke*; Otsuka, Takaharu*; Chazono, Yoshiki*; Hagen, G.*; Holt, J. D.*; et al.

Physics Letters B, 843, p.138025_1 - 138025_7, 2023/08

https://doi.org/10.1016/j.physletb.2023.138025

Gamma decays were observed in Ca and Ca following quasi-free one-proton knockout reactions from Sc. For Ca, a ray transition was measured to be 1456(12) keV, while for Ca an indication for a transition was observed at 1115(34) keV. Both transitions were tentatively assigned as the decays. A shell-model calculation in a wide model space with a marginally modified effective nucleon-nucleon interaction depicts excellent agreement with experiment for level energies, two-neutron separation energies, and reaction cross sections, corroborating the formation of a new nuclear shell above the N = 34 shell. Its constituents, the and orbitals, are almost degenerate. This degeneracy precludes the possibility for a doubly magic Ca and potentially drives the dripline of Ca isotopes to Ca or even beyond.

Multiple mechanisms in proton-induced nucleon removal at 100 MeV/nucleon

Pohl, T.*; Sun, Y. L.*; Obertelli, A.*; Lee, J.*; Gmez-Ramos, M.*; Ogata, Kazuyuki*; Yoshida, Kazuki; Cai, B. S.*; Yuan, C. X.*; Brown, B. A.*; et al.

Physical Review Letters, 130(17), p.172501_1 - 172501_8, 2023/04

https://doi.org/10.1103/PhysRevLett.130.172501

We report on the first proton-induced single proton- and neutron-removal reactions from the neutron deficient O nucleus with large Fermi-surface asymmetry at 100 MeV/nucleon. Our results provide the first quantitative contributions of multiple reaction mechanisms including the quasifree knockout, inelastic scattering, and nucleon transfer processes. It is shown that the inelastic scattering and nucleon transfer, usually neglected at such energy regime, contribute about 50% and 30% to the loosely bound proton and deeply bound neutron removal, respectively.

Extended neutron orbital and the shell closure in Ca

Enciu, M.*; Liu, H. N.*; Obertelli, A.*; Doornenbal, P.*; Nowacki, F.*; Ogata, Kazuyuki*; Poves, A.*; Yoshida, Kazuki; Achouri, N. L.*; Baba, Hidetada*; et al.

Physical Review Letters, 129(26), p.262501_1 - 262501_7, 2022/12

https://doi.org/10.1103/PhysRevLett.129.262501

The one-neutron knockout from Ca was performed at 230 MeV/nucleon combined with prompt spectroscopy. The momentum distributions corresponding to the removal of and neutrons were measured. The cross sections are consistent with a shell closure at the neutron number , found as strong as at and in Ca isotopes from the same observables. The analysis of the momentum distributions leads to a difference of the root-mean-square radii of the neutron and orbitals of 0.61(23) fm, in agreement with the modified-shell-model prediction of 0.7 fm suggesting that the large root-mean-square radius of the orbital in neutron-rich Ca isotopes is responsible for the unexpected linear increase of the charge radius with the neutron number.

The Translational, rotational, and phonon dynamics of water in ZrO/water nanofluid

Yoshida, Koji*; Sanada, Yusuke*; Yamaguchi, Toshio*; Matsuura, Masato*; Tamatsukuri, Hiromu; Uchiyama, Hiroshi*

Journal of Molecular Liquids, 366, p.120218_1 - 120218_9, 2022/11

https://doi.org/10.1016/j.molliq.2022.120218

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

https://doi.org/10.1016/j.molliq.2021.118080

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.

Pairing forces govern population of doubly magic Ca from direct reactions

Browne, F.*; Chen, S.*; Doornenbal, P.*; Obertelli, A.*; Ogata, Kazuyuki*; Utsuno, Yutaka; Yoshida, Kazuki; Achouri, N. L.*; Baba, Hidetada*; Calvet, D.*; et al.

Physical Review Letters, 126(25), p.252501_1 - 252501_7, 2021/06

https://doi.org/10.1103/PhysRevLett.126.252501

Direct proton-knockout reactions of Sc were studied at the RIKEN Radioactive Isotope Beam Factory. Populated states of Ca were investigated through -ray and invariant-mass spectroscopy. Level energies were calculated from the nuclear shell model employing a phenomenological inter-nucleon interaction. Theoretical cross sections to states were calculated from distorted-wave impulse approximation estimates multiplied by the shell model spectroscopic factors. Despite the calculations showing a significant amplitude of excited neutron configurations in the ground-state of Sc, valence proton removals populated predominantly the ground-state of Ca. This counter-intuitive result is attributed to pairing effects leading to a dominance of the ground-state spectroscopic factor. Owing to the ubiquity of the pairing interaction, this argument should be generally applicable to direct knockout reactions from odd-even to even-even nuclei.

The Impact of nuclear shape on the emergence of the neutron dripline

Tsunoda, Naofumi*; Otsuka, Takaharu; Takayanagi, Kazuo*; Shimizu, Noritaka*; Suzuki, Toshio*; Utsuno, Yutaka; Yoshida, Sota*; Ueno, Hideki*

Nature, 587, p.66 - 71, 2020/11

https://doi.org/10.1038/s41586-020-2848-x

no abstracts in English

The Effect of alkyl ammonium ionic liquids on thermal denaturation aggregation of -lactoglobulin

Yoshida, Koji*; Zenin, Tomohiro*; Fujiyoshi, Ayako*; Sanada, Yusuke*; Yamaguchi, Toshio*; Murata, Kunihiko*; Takata, Shinichi; Hiroi, Kosuke; Takahiro, Takekiyo*; Yoshimura, Yukihiro*

Journal of Molecular Liquids, 293, p.111477_1 - 111477_9, 2019/11

https://doi.org/10.1016/j.molliq.2019.111477

Ion hydration and association in an aqueous calcium chloride solution in the GPa range

Yamaguchi, Toshio*; Nishino, Masaaki*; Yoshida, Koji*; Takumi, Masaharu*; Nagata, Kiyofumi*; Hattori, Takanori

European Journal of Inorganic Chemistry, 2019(8), p.1170 - 1177, 2019/02

https://doi.org/10.1002/ejic.201900016

Neutron diffraction measurements of an aqueous 2 mol dm CaCl solutions in DO have been made at 1 GPa, 298 K as well as 0.1 MPa, 298 K. The experimental structure factors are subjected to Empirical Potential Structure Refinement (EPSR) modeling to reveal the ion hydration and association and solvent water at the atomic level. About seven water molecules surround Ca at the Ca-O and Ca-D distances of 2.44 and 3.70 , respectively, at both pressures, suggesting no significant pressure effect on the cation hydration. On the other hand, the Cl ion shows a drastic change in water oxygen coordination from 7 at 0.1 MPa to 14 at 1 GPa, accompanied by shortening of Cl-O distance from 3.18 to 3.15 . However, the number of water hydrogen atoms around Cl does not change significantly as 6.0 6.7 with shortening Cl-D distance from 2.22 to 2.18 on compression. The pressure effect on the solvent water structure is also drastic as an increase in water oxygen atoms of 4.7 at the O-O distance of 2.79 at 0.1 MPa to 10.3 at 2.85 at 1 GPa. The number of water hydrogen atoms, however, does not change as 1.2 at the O-D distance of 1.74 for both pressures, demonstrating the presence of the OD hydrogen bonds which are significantly bent at 1 GPa at 298 K. This change of hydrogen bonds in water with pressure probably causes the drastic increase in water oxygen atoms around Cl.