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Noguchi, Yoshifumi*; Hiyama, Miyabi*; Shiga, Motoyuki; Akiyama, Hidefumi*; Sugino, Osamu*
Journal of Chemical Physics, 153(20), p.201103_1 - 201103_6, 2020/11
Times Cited Count：2 Percentile：11.43(Chemistry, Physical)Stabilizing mechanisms of three isomers of the aqueous oxyluciferin in the first excited state were investigated using first-principles molecular dynamics simulations. Only the phenolate-keto isomer became attracted to the water molecules in its excited state and was stabilized by increasing the number of hydrogen bonds with nearby water molecules. The most stable isomer in the excited state was the phenolate-keto, and the phenolate-enol and phenol-enolate isomers were higher in energy by 0.38 eV and 0.57 eV, respectively, than the phenolate-keto. This was in contrast to the case of ground state in which the phenolate-enol was the most stable isomer.
Yan, L.*; Yamamoto, Yoshiyuki*; Shiga, Motoyuki; Sugino, Osamu*
Physical Review B, 101(16), p.165414_1 - 165414_9, 2020/04
Times Cited Count：11 Percentile：60.64(Materials Science, Multidisciplinary)Nuclear quantum effect and many-body interaction importantly interplay in the hydrogen on the Pt(111) system under the high coverage conditions of electrochemical interest, as revealed by our ab initio path integral and ring polymer molecular dynamics simulations done at room temperature. At the full monolayer coverage, hydrogen atoms are close-packed either at the atop sites or the fcc sites owing to their strong repulsion and the nearly degenerate nature of the adsorption sites. While at the 2/3 monolayer, they are delocalized over the fcc and hcp sites via the bridge sites because of the hopping. The quantum many-body effect is thus crucially important in determining the coverage dependence and provides a clue for reconciling the long-standing controversy on this system.
Hiyama, Miyabi*; Shiga, Motoyuki; Koga, Nobuaki*; Sugino, Osamu*; Akiyama, Hidefumi*; Noguchi, Yoshifumi*
Physical Chemistry Chemical Physics, 19(15), p.10028 - 10035, 2017/04
Times Cited Count：7 Percentile：31.12(Chemistry, Physical)In this study, the effect of hydration on the absorption spectra of oxyluciferin anion isomers in an aqueous solution is investigated for elucidating the influence of characteristic hydration structures. Using a canonical ensemble of hydration structures obtained from first-principles molecular dynamics simulations, the instantaneous absorption spectra of keto-, enol-, and enolate-type aqueous oxyluciferin anions at room temperature are computed from a collection of QM/MM calculations using an explicit solvent. It is demonstrated that the calculations reproduce experimental results concerning spectral shifts and broadening, for which traditional methods based on quantum chemistry and the Franck-Condon approximation fail because of the molecular vibrations of oxyluciferin anions and dynamical fluctuations of their hydration structures.
Noguchi, Yoshifumi*; Hiyama, Miyabi*; Shiga, Motoyuki; Sugino, Osamu*; Akiyama, Hidefumi*
Journal of Physical Chemistry B, 120(34), p.8776 - 8783, 2016/09
Times Cited Count：6 Percentile：15.29(Chemistry, Physical)We investigated the stability of oxyluciferin anions (keto, enol, and enolate isomers) in aqueous solution at room temperature by performing a nanosecond time scale first-principles molecular dynamics simulation. In contrast to all previous quantum chemistry calculations, which suggested the keto-type to be the most stable, we show that the enol-type is slightly more stable than the keto-type, in agreement with some recent experimental studies. The simulation highlights the remarkable hydrophobicity of the keto-type by the cavity formed at the oxyluciferin-water interface as well as a reduction in hydrophobicity with the number of hydrating water molecules. It is therefore predicted that the isomeric form in a hydrated cluster is size-dependent.
Konomura, Mamoru; Ogawa, Takashi; Okano, Yasushi; Yamaguchi, Hiroyuki; Murakami, Tsutomu; Takaki, Naoyuki; Nishiguchi, Youhei; Sugino, Kazuteru; Naganuma, Masayuki; Hishida, Masahiko; et al.
JNC TN9400 2004-035, 2071 Pages, 2004/06
JNC-TN9400-2004-035.pdf:76.42MB
The attractive concepts for Sodium-, lead-bismuth-, helium- and water-cooled FBRs have been created through using typical plant features and employing advanced technologies. Efforts on evaluating technological prospects of feasibility have been paid for these concepts. Also, it was comfirmed if these concepts satisfy design requierments of capability and performance presumed in the feasibilty study on commertialization of Fast Breeder Reactor Systems. As results, it was concluded that the selection of sodium-cooled reactor was most rational for practical use of FBR technologies in 2015.
