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Tsuji, Hayato*; Nakahata, Masaki*; Hishida, Mafumi*; Seto, Hideki*; Motokawa, Ryuhei; Inoue, Takeru*; Egawa, Yasunobu*
Journal of Physical Chemistry Letters (Internet), 14(49), p.11235 - 11241, 2023/12
Times Cited Count：0 Percentile：0.01(Chemistry, Physical)
neutron diffractionKobayashi, 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：1 Percentile：0.01(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 powder neutron diffraction experiments for DCl-doped D
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.
Kumada, Takayuki; Nakagawa, Hiroshi; Miura, Daisuke; Sekine, Yurina; Motokawa, Ryuhei; Hiroi, Kosuke; Inamura, Yasuhiro; Oku, Takayuki; Oishi, Kazuki*; Morikawa, Toshiaki*; et al.
Journal of Physical Chemistry Letters (Internet), 14(34), p.7638 - 7643, 2023/08
Times Cited Count：0 Percentile：0.01(Chemistry, Physical)The structure of nano-ice crystals in rapidly frozen glucose solution was elucidated by using spin-contrast-variation small-angle neutron scattering, which distinguishes the nano-ice crystal signal from the frozen amorphous solution signal by the polarization-dependent neutron scattering. The analysis revealed that the nano-ice crystals form a planar structure with a diameter exceeding tens of nanometers and a thickness of 1 nm, which is close to the critical nucleation size. This result suggests that the glucose molecules are preferentially bound to a specific face of nano-ice crystals, and then block the crystal growth perpendicular to that face.
ortho-para conversion on a metal surface; Interplay between electron and phonon systemsUeta, Hirokazu; Fukutani, Katsuyuki
Journal of Physical Chemistry Letters (Internet), 14(34), p.7591 - 7596, 2023/08
Times Cited Count：1NH and CaNH thin films by reactive magnetron sputtering under hydrogen partial pressure controlChon, S.*; Fukutani, Katsuyuki; 8 of others*
Journal of Physical Chemistry Letters (Internet), 13(43), p.10169 - 10174, 2022/11
Times Cited Count：0 Percentile：0.01(Chemistry, Physical)Kusaka, Ryoji; Watanabe, Masayuki
Journal of Physical Chemistry Letters (Internet), 13(30), p.7065 - 7071, 2022/08
Times Cited Count：5 Percentile：67.52(Chemistry, Physical)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：6 Percentile：50.99(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.
Yamamoto, Naoki*; Kofu, Maiko; Nakajima, Kenji; Nakagawa, Hiroshi; Shibayama, Naoya*
Journal of Physical Chemistry Letters (Internet), 12(8), p.2172 - 2176, 2021/03
Times Cited Count：9 Percentile：67.44(Chemistry, Physical)Hydration water plays a crucial role for activating the protein dynamics required for functional expression. Yet, the details are not understood about how hydration water couples with protein dynamics. A temperature hysteresis of the ice formation of hydration water is a key phenomenon to understand which type of hydration water, unfreezable or freezable hydration water, is crucial for the activation of protein dynamics. Using neutron scattering, we observed a temperature-hysteresis phenomenon in the diffraction peaks of the ice of freezable hydration water, whereas protein dynamics did not show any temperature hysteresis. These results show that the protein dynamics is not coupled with freezable hydration water dynamics, and unfreezable hydration water is essential for the activation of protein dynamics.
at the structure factor primary peak and prepeakLuo, P.*; Zhai, Y.*; Leao, J. B.*; Kofu, Maiko; Nakajima, Kenji; Faraone, A.*; Zhang, Y.*
Journal of Physical Chemistry Letters (Internet), 12(1), p.392 - 398, 2021/01
Times Cited Count：4 Percentile：35.04(Chemistry, Physical)Using neutron spin-echo spectroscopy, we studied the microscopic structural relaxation of a prototypical network ionic liquid ZnCl at the structure factor primary peak and prepeak. The results show that the relaxation at the primary peak is faster than the prepeak and that the activation energy is 
% higher. A stretched exponential relaxation is observed even at temperatures well-above the melting point 
. Surprisingly, the stretching exponent shows a rapid increase upon cooling, especially at the primary peak, where it changes from a stretched exponential to a simple exponential on approaching the . These results suggest that the appearance of glassy dynamics typical of the supercooled state even in the equilibrium liquid state of ZnCl as well as the difference of activation energy at the two investigated length scales are related to the formation of a network structure on cooling.
Ogawa, Shuichi*; Yamaguchi, Hisato*; Holby, E. F.*; Yamada, Takatoshi*; Yoshigoe, Akitaka; Takakuwa, Yuji*
Journal of Physical Chemistry Letters (Internet), 11(21), p.9159 - 9164, 2020/11
Times Cited Count：3 Percentile：17.73(Chemistry, Physical)Atomically thin layers of graphene have been proposed to protect surfaces through the direct blocking of corrosion reactants such as oxygen with low added weight. The long term efficacy of such an approach, however, is unclear due to the long-term desired protection of decades and the presence of defects in as-synthesized materials. Here, we demonstrate catalytic permeation of oxygen molecules through previously-described impermeable graphene by imparting sub-eV kinetic energy to molecules. These molecules represent a small fraction of a thermal distribution thus this exposure serves as an accelerated stress test for understanding decades-long exposures. The permeation rate of the energized molecules increased 2 orders of magnitude compared to their non-energized counterpart. Graphene maintained its relative impermeability to non-energized oxygen molecules even after the permeation of energized molecules indicating that the process is non-destructive and a fundamental property of the exposed material.
Gonzal
z, 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
Times Cited Count：17 Percentile：78.45(Chemistry, Physical)/Y
Fe
O
layers via longitudinal spin Seebeck effectLee, W.-Y.*; Park, N.-W.*; Kang, M.-S.*; Kim, G.-S.*; Jang, H. W.*; Saito, Eiji; Lee, S.-K.*
Journal of Physical Chemistry Letters (Internet), 11(13), p.5338 - 5344, 2020/07
Times Cited Count：11 Percentile：62.94(Chemistry, Physical)Fujiwara, Satoru*; Matsuo, Tatsuhito*; Sugimoto, Yasunobu*; Shibata, Kaoru
Journal of Physical Chemistry Letters (Internet), 10(23), p.7505 - 7509, 2019/12
Times Cited Count：4 Percentile：21.35(Chemistry, Physical)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.
Shiga, Motoyuki; Tuckerman, M. E.*
Journal of Physical Chemistry Letters (Internet), 9(21), p.6207 - 6214, 2018/11
Times Cited Count：4 Percentile：17.57(Chemistry, Physical)Predicting reaction pathways is one of the most important goals in theoretical and computational chemistry. In this paper, we propose a novel approach to search for free-energy landmarks, i.e., minima and the saddle points, of chemical reactions in an automated manner using a combination of steepest descent and gentlest ascent methods. As demonstrations, we present applications to the ring-opening reaction of benzocyclobutene and an SN2 reaction in aqueous solution.
Avramov, P.; Fedorov, D. G.*; Sorokin, P. B.*; Sakai, Seiji; Entani, Shiro; Otomo, Manabu; Matsumoto, Yoshihiro; Naramoto, Hiroshi*
Journal of Physical Chemistry Letters (Internet), 3(15), p.2003 - 2008, 2012/08
Times Cited Count：37 Percentile：79.31(Chemistry, Physical)Muroya, Yusa*; Lin, M.; De Waele, V.*; Hatano, Yoshihiko; Katsumura, Yosuke; Mostafavi, M.*
Journal of Physical Chemistry Letters (Internet), 1(1), p.331 - 335, 2010/01
Times Cited Count：43 Percentile：81.54(Chemistry, Physical)For the first time, a set-up is performed to carry out picoseconds time-resolved experiments in Supercritical Water (SCW) by pulse radiolysis. The kinetics of the decay of the hydrated electron is measured by transient absorption in the near IR on a time-scale ranging from 50 ps to 6 ns. The decay of the hydrated electrons in supercritical conditions shows a fast component at a short time below 500 ps, depending on the density of SCW. The results show that in SCW the main reaction for the decay of hydrated electron is that with HO
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