量子多成分系分子理論の深化と物質デザインへの展開

• Project Area: Materials Design through Computics: Complex Correlation and Non-equilibrium Dynamics
• Project/Area Number: 23104513
• Research Category: Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)
• Allocation Type: Single-year Grants
• Review Section: Science and Engineering
• Research Institution: Yokohama City University
• Principal Investigator: 立川 仁典 横浜市立大学, 生命ナノシステム科学研究科, 教授 (00267410)
• Project Period (FY): 2011-04-01 – 2013-03-31
• Project Status: Completed (Fiscal Year 2012)
• Budget Amount: ¥3,900,000 (Direct Cost: ¥3,000,000、Indirect Cost: ¥900,000); Fiscal Year 2012: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000); Fiscal Year 2011: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
• Keywords: 量子多成分系分子理論 / プロトン / ミューオン / 炭素材料への水素吸着 / 生体分子クラスター

Outline of Annual Research Achievements

これまで我々は、従来の第一原理計算だけでは直接取込むことのできない、水素原子核やミューオン、陽電子の量子揺らぎも含めた量子多成分系分子理論を展開してきた。具体的には、分子軌道(MO)法や、量子モンテカルロ(QMC)法、さらには密度汎関数(DFT)法に基づく手法と、経路積分法に基づいた、量子多成分系分子理論手法である。本研究課題では、このような量子多成分系分子理論を深化させ、計算機科学との融合を含めて、物質デザインへの展開を探る。本年度は、以下に示す研究項目を実施した。

①量子多成分系分子理論の深化：大規模系への拡張のため、経路積分法におけるポテンシャルの評価に、半経験的分子軌道法やDFTB法を実装することで計算コストを抑えることに成功した。併せて経路積分法における並列技法への実装も行った。それらの開発により、より効率的に計算を実施することを可能とした。
②物質デザインへの展開：①で開発した大規模計算可能な手法を駆使することにより、本年度は(1)経路積分分子動力学法を用いた核酸塩基対の水素結合における量子効果および温度効果による影響、および(2)ミューオン化合物の超微細結合定数に関する、予備的な解析を行った。
(1)G-C、A-T pairsに対しては150～450Kの温度条件で、分子軌道計算、古典分子動力学計算、経路積分分子動力学計算を実行した。主成分分析を行ったところ、最も低い四つの振動モード(buckle, propeller, opening, stagger)に対応する主成分が得られた。特に、核の量子効果はpropellerの分子振動を促進させることがわかった。

Research Progress Status

24年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

24年度が最終年度であるため、記入しない。

Research Products

• [Journal Article] Path integral molecular dynamic study of nuclear quantum effect on small chloride water clusters of Cl-(H2O)1-4 (2013)
  • Author(s): Q. Wang, K. Suzuki, U. Nagashima, M. Tachikawa, and S. Yan
  • Journal Title: Chem. Phys. Volume: in press
  • Peer Reviewed
• [Journal Article] Theoretical analysis of phase transition temperature of hydrogen-bonded dielectric materials induced by H/D isotope effec (2013)
  • Author(s): T. Ishimoto and M. Tachikawa
  • Journal Title: Progress in Theoretical Chemistry and Physics Volume: in press
  • Peer Reviewed
• [Journal Article] Quantum fluctuation and vibrational dynamics of aqueous Cu+ and Ag+ clusters (2013)
  • Author(s): A. Koizumi, M. Tachikawa, and M. Shiga
  • Journal Title: Chem. Phys. Volume: in press
  • Peer Reviewed
• [Journal Article] Semiempirical investigations on the stabilization energies and ionic hydrogen-bonded structures of F-(H2O)n and Cl-(H2O)n (n=1-4) clusters (2013)
  • Author(s): Q. Wang, K. Suzuki, U. Nagashima, M. Tachikawa, and S. Yan
  • Journal Title: J. Theoret. Appl. Phys. Volume: in press
  • Peer Reviewed
• [Journal Article] Theoretical analysis of the geometrical isotope effect on the hydrogen bonds in photoactive yellow protein with muti-component density functional theory (2013)
  • Author(s): Y. Kita, H. Kamikubo, M. Kataoka, and M. Tachikawa
  • Journal Title: Chem. Phys. Volume: in press
  • Peer Reviewed
• [Journal Article] Gold-standard coupled-cluster study of the ground-state chromium dimer cation (2013)
  • Author(s): Y. Yamada, K. Hongo, K. Egashira, Y. Kita, U. Nagashima, and M. Tachikawa
  • Journal Title: Chem. Phys. Lett. Volume: 555 Pages: 84-86
  • Peer Reviewed
• [Journal Article] Theoretical analysis of correlation between ionization threshold fluence in IR-MALDI and IR absorption spectrum of matrix molecules (2012)
  • Author(s): M. Hatakeyama, T. Mashiko, H. Hazama, K. Awazu, and M. Tachikawa
  • Journal Title: Int. J. Quant. Chem. Volume: 113 Pages: 125-129
  • Peer Reviewed
• [Journal Article] Theoretical Study on the Phase Transition and the H/D Isotope Effect of Squaric Acid (2012)
  • Author(s): T. Ishimoto and M. Tachikawa
  • Journal Title: Ferroics and Multiferroics (Periodical of Solid State Phenomena) Volume: 189 Pages: 169-177
  • Peer Reviewed
• [Journal Article] Theoretical Study on Isotope Effect for Phase Transition Temperature of Mixed K3H1-xDx(SO4)2, Mixed (H1-xDx)2SQ, Tritiated TKHS, and T2SQ Crystals (2012)
  • Author(s): T. Ishimoto and M. Tachikawa
  • Journal Title: Ferroelectrics Volume: 433 Pages: 170-179
  • Peer Reviewed
• [Journal Article] Ab initio path integral molecular dynamics simulations of F2H- and F2H3+ (2012)
  • Author(s): K. Suzuki, H. Ishibashi, K. Yagi, M. Shiga, and M. Tachikawa
  • Journal Title: Progress in Theoretical Chemistry and Physics Volume: B26 Pages: 207-216
  • Peer Reviewed
• [Journal Article] Vibrational enhancement of positron affinities for nonpolar carbon dioxide and carbon disulfide molecules: Multi- component molecular orbital study for vibrational excited states (2012)
  • Author(s): K. Koyanagi, Y. Kita, and M. Tachikawa
  • Journal Title: Int. J. Quant. Chem. Volume: 113 Pages: 382-385
  • Peer Reviewed
• [Journal Article] Temperature dependence of self-assembled molecular capsules consisting of gear-shaped amphiphile molecules with molecular dynamics simulations (2012)
  • Author(s): J. Koseki, Y. Kita, S. Hiraoka, U. Nagashima, and M. Tachikawa
  • Journal Title: Int. J. Quant. Chem. Volume: 113 Pages: 397-400
  • Peer Reviewed
• [Journal Article] Bound states of positron with simple carbonyl and aldehyde species with configuration interaction multi-component molecular orbital and local vibrational approaches (2012)
  • Author(s): M. Tachikawa, Y. Kita, and R. J. Buenker
  • Journal Title: New J. Phys. Volume: 14
  • Peer Reviewed
• [Journal Article] Systematic theoretical investigation of positron-binding to amino acid molecules with ab initio multi-component molecular orbital approach (2012)
  • Author(s): K. Koyanagi, Y. Kita, and M. Tachikawa
  • Journal Title: Eur. Phys. J. D Volume: 66
  • Peer Reviewed
• [Journal Article] Quantum tautomerization in porphycene and its isotopomers: Path-integral molecular dynamics simulations (2012)
  • Author(s): T. Yoshikawa, S. Sugawara, T. Takayanagi, M. Shiga, and M. Tachikawa
  • Journal Title: Chem. Phys. Volume: 394 Pages: 46-51
  • Peer Reviewed
• [Journal Article] Vibrational enhancement of positron affinities for nonpolar carbon dioxide and carbon disulfide molecules : Multi-component molecular orbital study for vibrational excited states (2012)
  • Author(s): K.Koyanagi, Y.Kita, M.Tachikawa
  • Journal Title: Int.J.Quant.Chem. Volume: (in press)
  • Peer Reviewed
• [Journal Article] Temperature dependence of self-assembled molecular capsules consisting of gear-shaped amphiphile molecules with molecular dynamics simulations (2012)
  • Author(s): J.Koseki, Y.Kita, S.Hiraoka, U.Nagashima, M.Tachikawa
  • Journal Title: Int.J.Quant.Chem. Volume: (in press)
  • Peer Reviewed
• [Journal Article] Bound states of positron with simple carbonyl and aldehyde species with configuration interaction multi-component molecular orbital and local vibrational approaches (2012)
  • Author(s): M.Tachikawa, Y.Kita, R.J.Buenker
  • Journal Title: New J.Phys. Volume: 14
  • Peer Reviewed
• [Journal Article] Systematic theoretical investigation of positron-binding to amino acid molecules with ab initio multi-component molecular orbital approach (2012)
  • Author(s): K.Koyanagi, Y.Kita, M.Tachikawa
  • Journal Title: Eur.Phys.J.D. Volume: (in press)
  • Peer Reviewed
• [Journal Article] Quantum tautomerization in porphycene and its isotopomers : Path-integral molecular dynamics simulations (2012)
  • Author(s): T.Yoshikawa, S.Sugawara, T.Takayanagi, M.Shiga, M Tachikawa
  • Journal Title: Chem.Phys. Volume: 394 Pages: 46-51
  • Peer Reviewed
• [Journal Article] Real Wave Packet and Flux Analysis Studies of the H+F_2->HF+F Reaction (2012)
  • Author(s): F.Gogtas, E.Karabulut, T.Takayanagi, T.Tanaka, R.Tutuk
  • Journal Title: Int.J.Quantum.Chem. Volume: (in press)
  • Peer Reviewed
• [Journal Article] Fixed-node quantum Monte Carlo for molecule (2012)
  • Author(s): 立川仁典, 北幸海
  • Journal Title: 巨大分子系の計算化学 Volume: (in Japanese) Pages: 34-38
  • Peer Reviewed
• [Journal Article] 陽電子束縛化合物の第一原理計算 (2012)
  • Author(s): 立川仁典, 北幸海
  • Journal Title: 日本物理学会誌 Volume: 67(in Japanese) Pages: 33-36
  • Peer Reviewed
• [Journal Article] Analytical optimization of orbital exponents in Gaussian-type functions for molecular systems based on MCSCF and MP2 levels of fully variational molecular orbital method (2011)
  • Author(s): N.Shimizu, T.Ishimoto, M.Tachikawa
  • Journal Title: Theor.Chem.Acc. Volume: 130 Pages: 679-685
  • Peer Reviewed
• [Journal Article] Role of CH-pi interaction energy in self-assembled gear-shaped amphiphile molecules : Correlated ab initio molecular orbital and density functional theory study (2011)
  • Author(s): J.Koseki, Y.Kita, S.Hiraoka, U.Nagashima, M.Tachikawa
  • Journal Title: Theor.Chem.Acc. Volume: 130 Pages: 1055-1059
  • Peer Reviewed
• [Journal Article] Quantum Proton Transfer in Hydrated Sulfuric Acid Clusters : A Perspective from Semiempirical Path Integral Simulations (2011)
  • Author(s): S.Sugawara, T.Yoshikawa, T.Takayanagi, M.Shiga, M.Tachikawa
  • Journal Title: J.Phys.Chem.A. Volume: 115 Pages: 11486-11494
  • Peer Reviewed
• [Journal Article] Isotope effect of proton and deuteron adsorption site on Zeolite-Templated carbon using path integral molecular dynamics (2011)
  • Author(s): K.Suzuki, M.Tachikawa, H.Ogawa, S.Ittisanronnachai, H.Nishihara, T.Kyotani, U.Nagashima
  • Journal Title: Theor.Chem.Acc. Volume: 130 Pages: 1039-1042
  • Peer Reviewed
• [Journal Article] Nuclear quantum effect on the hydrogen-bonded structure of guanine-cytosine pair (2011)
  • Author(s): M.Daido, A.Koizumi, M.Shiga, M.Tachikawa
  • Journal Title: Theor.Chem.Acc. Volume: 130 Pages: 385-391
  • Peer Reviewed
• [Journal Article] Ab initio quantum Monte Carlo study of the binding of a positron to alkali-metal hydrides (2011)
  • Author(s): Y.Kita, R.Maezono, M.Tachikawa, M.Towler, R.J.Needs
  • Journal Title: J.Chem.Phys. Volume: 135
  • Peer Reviewed
• [Journal Article] Ab initio path integral simulation of AgOH(H_2O) (2011)
  • Author(s): A.Koizumi, K.Suzuki, M.Shiga, M.Tachikawa
  • Journal Title: Int.J.Quant.Chem. Volume: 112 Pages: 136-139
  • Peer Reviewed
• [Journal Article] Theoretical study of the reversible photoconversion mechanism in Dronpa (2011)
  • Author(s): J.Koseki, Y.Kita, U.Nagashima, M.Tachikawa
  • Journal Title: Procedia Comput.Sci. Volume: 4 Pages: 251-260
  • Peer Reviewed
• [Journal Article] Molecular dynamics simulation for irreversible feature of green fluorescent protein before and after photoactivation (2011)
  • Author(s): J.Koseki, Y.Kita, M.Tachikawa
  • Journal Title: Chem.Lett. Volume: 40 Pages: 476-477
  • Peer Reviewed
• [Journal Article] Ab initio quantum chemical study on the mechanism of exceptional behavior of lysine for ion yields in MALDI-Role of vibrational entropic contribution in thermally averaged proton affinities- (2011)
  • Author(s): M.Hatakeyama, M.Tachikawa
  • Journal Title: J.Mass Spectrometry Volume: 46 Pages: 376-382
  • Peer Reviewed
• [Journal Article] Path integral molecular dynamics for hydrogen adsorption site of zeolite-templated carbon with semi-empirical PM3 potential (2011)
  • Author(s): K.Suzuki, M.Kayanuma, M.Tachikawa, H.Ogawa, H.Nishihara, T.Kyotani, U.Nagashima
  • Journal Title: Comp.Theor.Chem. Volume: 975 Pages: 128-133
  • Peer Reviewed
• [Journal Article] Nuclear quantum effect on the dissociation energies of cationic hydrogen clusters (2011)
  • Author(s): M.Sugimoto, M.Shiga, M.Tachikawa
  • Journal Title: Comp.Theor.Chem. Volume: 975 Pages: 31-37
  • Peer Reviewed
• [Journal Article] Theoretical investigations of nuclear quantum effect on molecular magnetic properties based on multi-component density functional theory (2011)
  • Author(s): Y.Kita, M.Tachikawa
  • Journal Title: Comp.Theor.Chem. Volume: 975 Pages: 9-12
  • Peer Reviewed
• [Journal Article] A concerted mechanism between protron transfer of Zundel anion and displacement of counter cation (2011)
  • Author(s): A.Koizumi, K.Suzuki, M.Shiga, M.Tachikawa
  • Journal Title: J.Chem.Phys. Volume: 134(communication)
  • Peer Reviewed
• [Journal Article] Theoretical study on mechanisms of structural rearrangement and ionic dissociation in the HCl(H_2O)_4 cluster with path-integral molecular dynamics simulations (2011)
  • Author(s): S.Sugawara, T.Yoshikawa, T.Takayanagi, M.Tachikawa
  • Journal Title: Chem.Phys.Lett. Volume: 501 Pages: 238-244
  • Peer Reviewed
• [Journal Article] Bound states of positron with nitrile species with configuration interaction multi-component molecular orbital approach (2011)
  • Author(s): M.Tachikawa, Y.Kita, R.J.Buenker
  • Journal Title: Phys.Chem.Chem.Phys. Volume: 13 Pages: 2701-2705
  • Peer Reviewed
• [Journal Article] Nuclear quantum effect on hydrogen adsorption site of zeolite-templated carbon model using path integral molecular dynamics (2011)
  • Author(s): K.Suzuki, M.Kayanuma, M.Tachikawa, H.Ogawa, H.Nishihara, T.Kyotani, U.Nagashima
  • Journal Title: J.Alloys and Compounds Volume: 509S
  • Peer Reviewed
• [Journal Article] 新しい分子物理化学の確立-ポジトロニクス(陽電子技術)にむけて (2011)
  • Author(s): 立川仁典, 北幸海
  • Journal Title: 化学 Volume: 66(最新のトピックス)(in Japanese) Pages: 68-69
  • Peer Reviewed
• [Presentation] Path Integral Simulation for Hydrogen Bondes Systems: Protonic Quantum Nature (2013)
  • Author(s): Masanori Tacihkawa
  • Organizer: Pure and Applied Chemistry International Conference 2013
  • Place of Presentation: The Tide Resort, Bangsaen Beachタイ（チョンブリー）
  • Invited
• [Presentation] Bound states of positron with nitrile species with several multi-component molecular theories (2012)
  • Author(s): Masanori Tachikawa
  • Organizer: International Workshop on Positrons in Astrophysics
  • Place of Presentation: Murren, Switzerland
  • Year and Date: 2012-03-21
• [Presentation] Multi component molecular theory for hydrogen bonded systems and positronic compounds (2012)
  • Author(s): Masanori Tachikawa
  • Organizer: The 4th French-Japanese Workshop on Computational Methods in Chemistry
  • Place of Presentation: Fukuoka, Japan(招待講演)
  • Year and Date: 2012-03-06
• [Presentation] First-principles Calculations for Positron-attached Molecules (2012)
  • Author(s): Masanori Tachikawa
  • Organizer: The Sixth General Meeting of ACCMS-VO
  • Place of Presentation: Sendai, Japan(招待講演)
  • Year and Date: 2012-02-12
• [Presentation] Multi-component molecular methods for hydrogen bonded systems and positronic compounds (2012)
  • Author(s): Masanori Tacihkawa
  • Organizer: XVIIth International Workshop on Quantum Systems in Chemistry and Physics (QSCP-XVII)
  • Place of Presentation: フィンランド（トゥルク）
  • Invited
• [Presentation] Multi-component molecular methods for hydrogen bonded systems and positronic compounds (2012)
  • Author(s): Masanori Tacihkawa
  • Organizer: 10th Asian International Seminar on Atomic and Molecular Physics
  • Place of Presentation: 台湾（台北）
  • Invited
• [Presentation] Multi Component Molecular Theory for Hydrogen Bonded Systems and Positronic Compounds (2012)
  • Author(s): Masanori Tacihkawa
  • Organizer: The Sevenh General Meeting of ACCMS-VO
  • Place of Presentation: 東北大学（宮城県）
  • Invited
• [Presentation] Multi component molecular theory for hydrogen bonded systems and positronic compounds (2011)
  • Author(s): Masanori Tachikawa
  • Organizer: XVIth International Workshop on Quantum Systems in Chemistry and Physics (QSCP-XVI)
  • Place of Presentation: Kanazawa, Ishikawa(招待講演)
  • Year and Date: 2011-09-14
• [Presentation] Path Integral simulation for Hydrogen Bonded Systems : Protonic Quantum Nature and H/D Isotope Effect (2011)
  • Author(s): Masanori Tachikawa
  • Organizer: 14th Asian Chemical Congress
  • Place of Presentation: Bangkok, Thailand(招待講演)
  • Year and Date: 2011-09-08
• [Presentation] Multi component molecular theory for hydrogen bonded systems and positronic compounds (2011)
  • Author(s): Masanori Tachikawa
  • Organizer: 7th Congress of the International Society for Theoretical Chemical Physics (ISTCP-VII)
  • Place of Presentation: Waseda, Tokyo
  • Year and Date: 2011-09-04
• [Presentation] Path integral simulation for hydrogen bonded systems : Protonic quantum nature and H/D isotope effect (2011)
  • Author(s): Masanori Tachikawa
  • Organizer: ISOTOPES2011
  • Place of Presentation: Provence-Alpes-Cote d'Azur, FRANCE(招待講演)
  • Year and Date: 2011-06-22
• [Remarks] 横浜市立大学大学院生命ナノシステム科学研究科量子物理化学研究室
  • URL: http://www-user.yokohama-cu.ac.jp/~tachi/
• [Remarks]
  • URL: http://www-user.yokohama-cu.ac.jp/~tachi/