Organization of malonamides from the interface to the organic bulk phase

Micheau, C.; Ueda, Yuki; Motokawa, Ryuhei; Akutsu, Kazuhiro*; Yamada, Norifumi*; Yamada, Masako*; Moussaoui, S. A.*; Makombe, E.*; Meyer, D.*; Berthon, L.*; et al.

Journal of Molecular Liquids, 401, p.124372_1 - 124372_12, 2024/05

https://doi.org/10.1016/j.molliq.2024.124372

Supramolecular organization of extractant molecules impacts metal ions separation behavior. Probing bulk and interfacial structures of the relevant systems is expected to provide key insights into the metal ion selectivity and kinetic aspects. The supramolecular features of two solvent extraction systems based on malonamide extractants THMA in toluene and DBMA in n-heptane were studied using small-angle X-ray scattering for the organic bulk phases, as well as interfacial tension and neutron reflectivity measurements for the interfaces. In the bulk solution, THMA forms dimeric/trimeric associates but no aggregates in toluene, while DBMA forms large aggregates in n-heptane. On the other hand, THMA accumulates in a diffuse layer at the interface at high THMA concentration, whereas DBMA forms a compact but thinner layer. After Pd(II) extraction, the thickness of interfacial layers decreases in the case of THMA, and totally vanishes in the case of DBMA. Based on these new structural information, two mechanisms are proposed for Pd(II) and Nd(III) extraction with malonamides. In toluene, THMA associates slightly accumulate in the vicinity of the interface, then coordinate Pd(II) and diffuse into the organic bulk phase. In n-heptane, DBMA aggregates adsorb at the interface then pick up Nd(III) cations in their polar cores and finally diffuse into the bulk.

Quantum critical behavior of the hyperkagome magnet MnCoSi

Yamauchi, Hiroki; Sari, D. P.*; Yasui, Yukio*; Sakakura, Terutoshi*; Kimura, Hiroyuki*; Nakao, Akiko*; Ohara, Takashi; Honda, Takashi*; Kodama, Katsuaki; Igawa, Naoki; et al.

Physical Review Research (Internet), 6(1), p.013144_1 - 013144_9, 2024/02

https://doi.org/10.1103/PhysRevResearch.6.013144

New measurement system based on small-angle neutron scattering for structural analysis of light-responsive materials

Iwase, Hiroki*; Akamatsu, Masaaki*; Inamura, Yasuhiro; Sakaguchi, Yoshifumi*; Morikawa, Toshiaki*; Kasai, Satoshi*; Ouchi, Keiichi*; Kobayashi, Kazuki*; Sakai, Hideki*

Journal of Applied Crystallography, 56(1), p.110 - 115, 2023/02

https://doi.org/10.1107/S1600576722011104

With the increasing importance of light-responsive materials, it is vital to analyze the relationship between function and structural changes induced by light irradiation. Small-angle scattering (SAS) is effective for such structural analysis. However, quantitatively capturing local molecular structure formation and molecular reactions at a scale of less than 1 nm via SAS is difficult. In this study, to analyze the structure of non-equilibrium phenomena in light-responsive materials, a new sample environment has been developed for a time-of-flight small- and wide-angle neutron scattering instrument (TAIKAN), comprising a UV-Vis irradiation system, UV-Vis absorption measurement equipment and photodetector. Simultaneous measurement of small-angle neutron scattering and UV-Vis absorption was achieved. This system was used to demonstrate the in situ observation of UV-Vis irradiation-induced structural change of micelles formed by a light-responsive surfactant sample in an aqueous solution.

Rotation of complex ions with ninefold hydrogen coordination studied by quasielastic neutron scattering and first-principles molecular dynamics calculations

Omasa, Yoshinori*; Takagi, Shigeyuki*; Toshima, Kento*; Yokoyama, Kaito*; Endo, Wataru*; Orimo, Shinichi*; Saito, Hiroyuki*; Yamada, Takeshi*; Kawakita, Yukinobu; Ikeda, Kazutaka*; et al.

Physical Review Research (Internet), 4(3), p.033215_1 - 033215_9, 2022/09

https://doi.org/10.1103/PhysRevResearch.4.033215

Multipole polaron in the devil's staircase of CeSb

Arai, Yosuke*; Kuroda, Kenta*; Nomoto, Takuya*; Tin, Z. H.*; Sakuragi, Shunsuke*; Bareille, C.*; Akebi, Shuntaro*; Kurokawa, Kifu*; Kinoshita, Yuto*; Zhang, W.-L.*; et al.

Nature Materials, 21(4), p.410 - 415, 2022/04

https://doi.org/10.1038/s41563-021-01188-9

Quartz cell for a backscattering spectrometer

Tominaga, Taiki*; Kawakita, Yukinobu; Nakagawa, Hiroshi; Yamada, Takeshi*; Shibata, Kaoru

JPS Conference Proceedings (Internet), 33, p.011086_1 - 011086_5, 2021/03

BB2019-1956.pdf:0.78MB

https://doi.org/10.7566/JPSCP.33.011086

We developed a quartz double cylindrical sample cell optimized for a backscattering neutron spectrometer, especially for BL02 (DNA), MLF in J-PARC. A quartz glass tube, with one end closed, is shaved to obtain a wall thickness of 0.55 mm. The inner tube is properly centered using a protrusion into the outer tube such that the interstice between the outer and inner tubes keeps constant. This quartz cell can be used for samples that should not be in contact with the aluminum surface. We verified cell's background effect between the quartz cell and Al cell by QENS measurements using DO buffer. The elastic intensity profiles of the buffer in a low Q region were identical between both quartz cell and Al cell (A1070). In a high Q region, however, the profiles were different caused by the first sharp diffraction peak of quartz glass. For this region the data should be analyzed by consideration of absorption correction and diffraction in individual thickness of quartz cell.

Nanoscale relaxation in "Water-in-Salt" and "Water-in-Bisalt" electrolytes

Gonzalz, M. A.*; Borodin, O.*; Kofu, Maiko; Shibata, Kaoru; Yamada, Takeshi*; Yamamuro, Osamu*; Xu, K.*; Price, D. L.*; Saboungi, M.-L.*

Journal of Physical Chemistry Letters (Internet), 11(17), p.7279 - 7284, 2020/09

https://doi.org/10.1021/acs.jpclett.0c01765

Segmental motions of proteins under non-native states evaluated using quasielastic neutron scattering

Fujiwara, Satoru*; Matsuo, Tatsuhito*; Sugimoto, Yasunobu*; Shibata, Kaoru

Journal of Physical Chemistry Letters (Internet), 10(23), p.7505 - 7509, 2019/12

https://doi.org/10.1021/acs.jpclett.9b03196

Characterization of the dynamics of disordered polypeptide chains is required to elucidate the behavior of intrinsically disordered proteins and proteins under non-native states related to the folding process. Here we develop a method using quasielastic neutron scattering, combined with small-angle X-ray scattering and dynamic light scattering, to evaluate segmental motions of proteins as well as diffusion of the entire molecules and local side-chain motions. We apply this method to RNase A under the unfolded and molten-globule (MG) states. The diffusion coefficients arising from the segmental motions are evaluated and found to be different between the unfolded and MG states. The values obtained here are consistent with those obtained using the fluorescence-based techniques. These results demonstrate not only feasibility of this method but also usefulness to characterize the behavior of proteins under various disordered states.

Local structure of functional solids

Shamoto, Shinichi

Journal of the Physical Society of Japan, 88(8), p.081008_1 - 081008_11, 2019/08

AA2019-0006.pdf:1.06MB

https://doi.org/10.7566/JPSJ.88.081008

Cryogenic sample environments shared at the MLF, J-PARC

Kawamura, Seiko; Takahashi, Ryuta*; Ishikado, Motoyuki*; Yamauchi, Yasuhiro*; Nakamura, Masatoshi*; Ouchi, Keiichi*; Kira, Hiroshi*; Kambara, Wataru*; Aoyama, Kazuhiro*; Sakaguchi, Yoshifumi*; et al.

Journal of Neutron Research, 21(1-2), p.17 - 22, 2019/05

https://doi.org/10.3233/JNR-190106

The Cryogenics and Magnets group in the Sample Environment team is responsible for operation of cryostats and magnets for user's experiments at the MLF in J-PARC. We have introduced a top-loading He cryostat, a bottom-loading He cryostat, a dilution refrigerator insert and a superconducting magnet. The frequency of use of them dramatically becomes higher in these two years, as the beam power and the number of proposal increase. To respond such situation, we have made efforts to enhance performance of these equipment as follows. The He cryostat originally involves an operation software for automatic initial cooling down to the base temperature and automatic re-charge of He. Recently we made an additional program for automatic temperature control with only the sorb heater. Last year, a new outer vacuum chamber of the magnet with an oscillating radial collimator (ORC) was fabricated. The data quality was drastically improved by introducing this ORC so that the magnet can be used even for the inelastic neutron scattering experiments.