Development of multicomponent quantum chemistry methods for accurate prediction and elucidation of hydrogen-functional mechanism

• Project Area: HYDROGENOMICS: Creation of Innovative Materials, Devices, and Reaction Processes using Higher-Order Hydrogen Functions
• Project/Area Number: 19H05063
• 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, データサイエンス学部, 教授 (00267410)
• Project Period (FY): 2019-04-01 – 2021-03-31
• Project Status: Completed (Fiscal Year 2020)
• Budget Amount: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000); Fiscal Year 2020: ¥1,690,000 (Direct Cost: ¥1,300,000、Indirect Cost: ¥390,000); Fiscal Year 2019: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000)
• Keywords: 多成分系量子化学手法 / 量子水素 / H/D同位体効果 / 低障壁水素結合

Outline of Research at the Start

材料中の水素が示す高次水素機能の発現機構解明および高精度予測のために、申請者が構築してきた量子化学計算手法を高度化させ、領域内での実験グループとの密な議論に基づきこの課題に挑戦する。具体的には、多成分系量子化学計算手法の高度化として、階層的手法や、効率的サンプリング手法等の導入を行う。それにより、低障壁水素結合に着目した高次水素機能の発現機構解明および高精度予測に向け、 分子性結晶や表面化学、さらには生体超分子に焦点を絞った大規模計算を実現する。

Outline of Annual Research Achievements

高次水素機能の発現機構解明および高精度予測を目指し、多成分系量子化学計算手法を高度化し、低障壁水素結合に着目した大規模計算を実現することを目標とする。この２年間で以下の研究項目を実現し、当該領域「ハイドロジェノミクス」の研究推進に貢献した。
研究項目１．多成分系量子化学計算システムに、拡張型ONIOM法を開発・実装し、実構造に近い計算を可能とした。具体的には、平面波基底と局在化基底の利点を組み合わせた「Combined Plane wave and Localized Basis-sets (CPLB)法」を開発し、金属表面上の局所的な高精度計算の可能性を示した。また、金属表面での構造緩和を取り込むために、CPLB法の枠組みにおいて構造最適化プログラムを実装した。本研究では吉信らのRh(111)に対するC6H12/C6D12吸着のH/D同位体効果の発現機構の解明に向け、CH4/CD4を例にとり吸着特性についての解析を行った。その結果、C-Rh(111)表面間距離はCD4の方が0.009Å長くなり、吉信らの吸着距離に対する実験報告と同様の傾向を示すことに成功した。
研究項目２．低障壁水素結合(LBHB)に着目した高次水素機能の発現機構解明および高精度予測にむけた大規模計算を実現した。森らの開発したLBHBを有するH3(Cat-EDT-TTF)2、およびその重水素置換化体に対する計算を実現し、さらには静電場を印加した計算を実現した。
以上の成果により第4回（2019年度）分子科学国際学術賞を受賞すると共に、１０報の査読付き国際誌に報告した。

Research Progress Status

令和2年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

令和2年度が最終年度であるため、記入しない。

Research Products

• [Int'l Joint Research] チェンマイ大学/ウボンラチャタニ大学(タイ)
• [Int'l Joint Research] チェンマイ大学/ウボンラチャタニ大学(タイ)
• [Journal Article] Development of anharmonic vibrational structure theory using backflow transformation (2022)
  • Author(s): Ishii Kiriko、Shimazaki Tomomi、Tachikawa Masanori、Kita Yukiumi
  • Journal Title: Chemical Physics Letters Volume: 787 Pages: 139263-139263
  • DOI: 10.1016/j.cplett.2021.139263
  • Peer Reviewed
• [Journal Article] Hydrogen/Deuterium Transfer from Anisole to Methoxy Radicals: A Theoretical Study of a Deuterium-Labeled Drug Model (2022)
  • Author(s): Kimura Yuka、Kanematsu Yusuke、Sakagami Hiroki、Rivera Rocabado David S.、Shimazaki Tomomi、Tachikawa Masanori、Ishimoto Takayoshi
  • Journal Title: The Journal of Physical Chemistry A Volume: 126 Issue: 1 Pages: 155-163
  • DOI: 10.1021/acs.jpca.1c08514
  • Peer Reviewed
• [Journal Article] Atomic mass dependence of the nuclear quantum effect in NH4+(H2O) (2022)
  • Author(s): Kuwahata Kazuaki、Tachikawa Masanori
  • Journal Title: Chemical Physics Volume: 553 Pages: 111381-111381
  • DOI: 10.1016/j.chemphys.2021.111381
  • Peer Reviewed
• [Journal Article] Spontaneous radiative dissociation of the second bound state of positronium hydride (2022)
  • Author(s): Yamashita Takuma、Hiyama Emiko、Yoshida Daisuke、Tachikawa Masanori
  • Journal Title: Physical Review A Volume: 105 Issue: 1 Pages: 012814-012814
  • DOI: 10.1103/physreva.105.012814
  • Peer Reviewed
• [Journal Article] Competitive nuclear quantum effect and H/D isotope effect on torsional motion of H2O2: An ab initio path integral molecular dynamics study (2022)
  • Author(s): Udagawa Taro、Kuwahata Kazuaki、Tachikawa Masanori
  • Journal Title: Computational and Theoretical Chemistry Volume: 1208 Pages: 113542-113542
  • DOI: 10.1016/j.comptc.2021.113542
  • Peer Reviewed
• [Journal Article] Theoretical study of the H/D isotope effect of CH4/CD4 adsorption on a Rh(111) surface using a combined plane wave and localized basis sets method (2021)
  • Author(s): Sakagami Hiroki、Tachikawa Masanori、Ishimoto Takayoshi
  • Journal Title: RSC Advances Volume: 11 Issue: 17 Pages: 10253-10257
  • DOI: 10.1039/d0ra10796d
  • Peer Reviewed / Open Access
• [Journal Article] Metal-doped carbon nanocones as highly efficient catalysts for hydrogen storage: Nuclear quantum effect on hydrogen spillover mechanism (2021)
  • Author(s): Yodsin Nuttapon、Sakagami Hiroki、Udagawa Taro、Ishimoto Takayoshi、Jungsuttiwong Siriporn、Tachikawa Masanori
  • Journal Title: Molecular Catalysis Volume: 504 Pages: 111486-111486
  • DOI: 10.1016/j.mcat.2021.111486
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] H/D Isotope Effects in Keto-Enol Tautomerism of β-Dicarbonyl Compounds: Importance of Nuclear Quantum Effects of Hydrogen Nuclei (2021)
  • Author(s): Udagawa Taro、Murphy Rhys B.、Darwish Tamim A.、Tachikawa Masanori、Mori Seiji
  • Journal Title: Bulletin of the Chemical Society of Japan Volume: 94 Issue: 7 Pages: 1954-1962
  • DOI: 10.1246/bcsj.20210083
  • NAID: 130008076866
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Theoretical investigation of the enhancement of positron affinity by the vibration and dimerization of non-polar carbon disulfide (2021)
  • Author(s): Furushima Miku、Yoshida Daisuke、Kita Yukiumi、Shimazaki Tomomi、Tachikawa Masanori
  • Journal Title: Physical Chemistry Chemical Physics Volume: 23 Issue: 38 Pages: 21512-21520
  • DOI: 10.1039/d1cp02808a
  • Peer Reviewed
• [Journal Article] A theoretical study on solvatofluorochromic asymmetric thiazolothiazole (TTz) dyes using dielectric-dependent density functional theory (2021)
  • Author(s): Shimazaki Tomomi、Tachikawa Masanori
  • Journal Title: Physical Chemistry Chemical Physics Volume: 23 Issue: 37 Pages: 21078-21086
  • DOI: 10.1039/d1cp02047a
  • Peer Reviewed
• [Journal Article] H/D isotope effect between adsorbed water (H2O, D2O, and HDO) and H2O- and D2O-ice Ih(0001) basal surfaces based on the combined plane wave and localized basis set method (2021)
  • Author(s): Ishimoto Takayoshi、Sakagami Hiroki、Kanematsu Yusuke、Tachikawa Masanori
  • Journal Title: Applied Surface Science Volume: 561 Pages: 150100-150100
  • DOI: 10.1016/j.apsusc.2021.150100
  • Peer Reviewed
• [Journal Article] Theoretical Study For Positron Binding and Annihilation of Alcohol Clusters (2021)
  • Author(s): Tachikawa Masanori、Yoshida Daisuke
  • Journal Title: Few-Body Systems Volume: 62 Issue: 3 Pages: 48-53
  • DOI: 10.1007/s00601-021-01636-x
  • Peer Reviewed
• [Journal Article] Positron Binding and Annihilation Properties of Amino Acid Systems (2021)
  • Author(s): Ozaki Maya、Yoshida Daisuke、Kita Yukiumi、Shimazaki Tomomi、Tachikawa Masanori
  • Journal Title: ACS Omega Volume: 6 Issue: 44 Pages: 29449-29458
  • DOI: 10.1021/acsomega.1c03409
  • Peer Reviewed / Open Access
• [Journal Article] Path Integral Molecular Dynamics Study on NH4+(H2O) (2021)
  • Author(s): Kuwahata Kazuaki、Tachikawa Masanori
  • Journal Title: Few-Body Systems Volume: 62 Issue: 4 Pages: 96-102
  • DOI: 10.1007/s00601-021-01689-y
  • Peer Reviewed
• [Journal Article] Contribution of vibrational overtone excitations to positron annihilation rates for benzene and naphthalene (2021)
  • Author(s): R. Iida, H. Suzuki, T. Takayanagi, M. Tachikawa
  • Journal Title: Phys. Rev. A Volume: 104 Issue: 6
  • DOI: 10.1103/physreva.104.062807
  • Peer Reviewed
• [Journal Article] Theoretical analysis of the binding of a positron and pair-annihilation in fluorinated benzene molecules (2020)
  • Author(s): Ono Kuniaki、Oyamada Takayuki、Kita Yukiumi、Tachikawa Masanori
  • Journal Title: The European Physical Journal D Volume: 74 Issue: 5 Pages: 1-8
  • DOI: 10.1140/epjd/e2020-100538-3
  • Peer Reviewed
• [Journal Article] Geometrical H/D Isotope Effect of Blue-shifting Dihydrogen-bonded Clusters (2020)
  • Author(s): Ishida Yusuke、Funahashi Haruki、Tachikawa Masanori、Udagawa Taro
  • Journal Title: Chemistry Letters Volume: 49 Issue: 6 Pages: 745-748
  • DOI: 10.1246/cl.200198
  • NAID: 130007852141
  • Peer Reviewed
• [Journal Article] Experimental and Computational Analyses of the Oxidation Mechanism of the Poly(arylsilane) Family as the Side Reaction during the Baking Process (2020)
  • Author(s): Kobayashi Osamu、Noda Kunihiro、Ikuma Naohiko、Shiota Dai、Ishimoto Takayoshi、Tachikawa Masanori
  • Journal Title: The Journal of Physical Chemistry C Volume: 124 Issue: 29 Pages: 16149-16158
  • DOI: 10.1021/acs.jpcc.0c02416
  • Peer Reviewed
• [Journal Article] Positron-electron correlation polarization potential model for positron binding in polyatomic molecules (2020)
  • Author(s): Y. Sugiura, H. Suzuki, T. Otomo, T. Miyazaki, T. Takayanagi, M. Tachikawa
  • Journal Title: J. Comp. Chem. Volume: 41 Issue: 17 Pages: 1576-1585
  • DOI: 10.1002/jcc.26200
  • Peer Reviewed
• [Journal Article] Hydrogen/deuterium adsorption and absorption properties on and in palladium using a combined plane wave and localized basis set method (2020)
  • Author(s): Hiroki Sakagami, Masanori Tachikawa, Takayoshi Ishimoto
  • Journal Title: International Journal of Quantum Chemistry Volume: 120 Issue: 16
  • DOI: 10.1002/qua.26275
  • Peer Reviewed
• [Journal Article] Determining if Reaction Selectivity Can Be Controlled by the H/D Isotope Effect in CH・・・O Interactions (2020)
  • Author(s): Funahashi Haruki、Tachikawa Masanori、Udagawa Taro
  • Journal Title: Organic Letters Volume: 22 Issue: 24 Pages: 9439-9443
  • DOI: 10.1021/acs.orglett.0c03351
  • Peer Reviewed
• [Journal Article] Theoretical calculation of positron annihilation spectrum using positron‐electron correlation‐polarization potential (2020)
  • Author(s): Y. Sugiura, T. Takayanagi, M. Tachikawa
  • Journal Title: Int. J. Quantum Chem. Volume: 120 Issue: 22
  • DOI: 10.1002/qua.26376
  • Peer Reviewed
• [Journal Article] Positron binding in chloroethenes: Modeling positron-electron correlation-polarization potentials for molecular calculations (2020)
  • Author(s): H. Suzuki, T. Otomo, R. Iida, Y. Sugiura, T. Takayanagi, M. Tachikawa
  • Journal Title: Phys. Rev. A Volume: 102 Issue: 5
  • DOI: 10.1103/physreva.102.052830
  • Peer Reviewed / Open Access
• [Journal Article] First-principles quantum Monte Carlo studies for prediction of double minima for positronic hydrogen molecular dianion (2020)
  • Author(s): Ito Shumpei、Yoshida Daisuke、Kita Yukiumi、Tachikawa Masanori
  • Journal Title: The Journal of Chemical Physics Volume: 153 Issue: 22 Pages: 224305-224305
  • DOI: 10.1063/5.0022673
  • Peer Reviewed
• [Journal Article] Nuclear Quantum Effect on the Geometry of NH4+(H2O) (2020)
  • Author(s): Kuwahata Kazuaki、Tachikawa Masanori
  • Journal Title: Bulletin of the Chemical Society of Japan Volume: 93 Issue: 12 Pages: 1558-1563
  • DOI: 10.1246/bcsj.20200120
  • NAID: 130007955871
  • Peer Reviewed
• [Journal Article] Computational simulation of anion binding association mechanisms contributing toward rotation of pyrrole rings in dipyrrolyldiketone BF2 complexes (2020)
  • Author(s): Kobayashi Osamu、Kato Tomoki、Mashiko Takako、Haketa Yohei、Maeda Hiromitsu、Tachikawa Masanori
  • Journal Title: RSC Advances Volume: 10 Issue: 20 Pages: 12013-12024
  • DOI: 10.1039/c9ra09285d
  • Peer Reviewed / Open Access
• [Journal Article] A computational examination of the electric-field-induced proton transfer along the interface hydrogen bond between proton donating and accepting self-assembled monolayers (2020)
  • Author(s): Kanematsu Yusuke、Kato Hiroyuki S.、Yoshimoto Shinya、Ueda Akira、Yamamoto Susumu、Mori Hatsumi、Yoshinobu Jun、Matsuda Iwao、Tachikawa Masanori
  • Journal Title: Chemical Physics Letters Volume: 741 Pages: 137091-137091
  • DOI: 10.1016/j.cplett.2020.137091
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Nuclear quantum and H/D isotope effects on three‐centered bonding diborane: Path integral molecular dynamics simulations (2020)
  • Author(s): Daengngern Rathawat、Kobayashi Osamu、Kungwan Nawee、Ngaojampa Chanisorn、Tachikawa Masanori
  • Journal Title: International Journal of Quantum Chemistry Volume: 120 Issue: 10
  • DOI: 10.1002/qua.26179
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Quantum dynamics calculation of the annihilation spectrum for positron-proline scattering (2019)
  • Author(s): Y. Sugiura, K. Suzuki, S. Koido, T. Takayanagi, Y. Kita, and M. Tachikawa
  • Journal Title: Comp. Theo. Chem. Volume: 1147 Pages: 1-7
  • DOI: 10.1016/j.comptc.2018.11.013
  • Peer Reviewed
• [Journal Article] Hydration effect on positron binding ability for proline: Positron attachment induces proton-transfer to form zwitterionic structure (2019)
  • Author(s): K. Suzuki, Y. Sugiura, T. Takayanagi, Y. Kita, and M. Tachikawa
  • Journal Title: J. Phys. Chem. A Volume: 123 Issue: 6 Pages: 1217-1224
  • DOI: 10.1021/acs.jpca.8b11653
  • Peer Reviewed
• [Journal Article] Theoretical Study on Hydrogen-Tritium Exchange Reactions between Several Organic and HTO Molecules: A Multicomponent QM Study (2019)
  • Author(s): Ishibashi Rina、Tachikawa Masanori、Udagawa Taro
  • Journal Title: Bulletin of the Chemical Society of Japan Volume: 92 Issue: 3 Pages: 592-599
  • DOI: 10.1246/bcsj.20180308
  • NAID: 130007611380
  • Peer Reviewed
• [Journal Article] Molecular Dynamics Study on Dynamical Features of Reorganization Process for Nanocapsule Formed with Gear-Shaped Amphiphile Molecules (2019)
  • Author(s): Mashiko Takako、Hiraoka Shuichi、Nagashima Umpei、Tachikawa Masanori
  • Journal Title: The Journal of Physical Chemistry B Volume: 123 Issue: 24 Pages: 5176-5180
  • DOI: 10.1021/acs.jpcb.9b02156
  • Peer Reviewed
• [Journal Article] Positron binding to hydrocarbon molecules: Calculation using the positron-electron correlation polarization potential (2019)
  • Author(s): Y. Sugiura, T. Takayanagi, Y. Kita, M. Tachikawa
  • Journal Title: Eur. Phys. J. D Volume: 73 Issue: 8 Pages: 1621-10
  • DOI: 10.1140/epjd/e2019-100147-y
  • Peer Reviewed
• [Journal Article] Quantum Stabilization of the Frustrated Hydrogen Bonding Structure in the Hydrogen Fluoride Trimer (2019)
  • Author(s): Io Aiko、Kawatsu Tsutomu、Tachikawa Masanori
  • Journal Title: The Journal of Physical Chemistry A Volume: 123 Issue: 37 Pages: 7950-7955
  • DOI: 10.1021/acs.jpca.9b04407
  • Peer Reviewed
• [Journal Article] Polarizability and isotope effects on dispersion interactions in water (2019)
  • Author(s): Zhan Yi-Yang、Jiang Qi-Chun、Ishii Kentaro、Koide Takuya、Kobayashi Osamu、Kojima Tatsuo、Takahashi Satoshi、Tachikawa Masanori、Uchiyama Susumu、Hiraoka Shuichi
  • Journal Title: Communications Chemistry Volume: 2 Issue: 1 Pages: 1-8
  • DOI: 10.1038/s42004-019-0242-0
  • Peer Reviewed
• [Journal Article] One-Dimensional Fullerene/Porphyrin Cocrystals: Near-Infrared Light Sensing through Component Interactions (2019)
  • Author(s): Wakahara Takatsugu、Nagaoka Kahori、Nakagawa Akari、Hirata Chika、Matsushita Yoshitaka、Miyazawa Kun’ichi、Ito Osamu、Wada Yoshiki、Takagi Makito、Ishimoto Takayoshi、Tachikawa Masanori、Tsukagoshi Kazuhito
  • Journal Title: ACS Applied Materials & Interfaces Volume: 12 Issue: 2 Pages: 2878-2883
  • DOI: 10.1021/acsami.9b18784
  • Peer Reviewed
• [Presentation] Ab initio study of the effect of molecular vibrations on the positron-binding to polyatomic molecules (2021)
  • Author(s): Masanori Tachikawa
  • Organizer: The 8th Asia-Pacific Conference on Few-Body Problems in Physics (APFB2020)
  • Int'l Joint Research / Invited
• [Presentation] エキゾチック分子の量子化学 (2021)
  • Author(s): 立川仁典
  • Organizer: IQCE量子化学探索講演会2021「量子化学で探る化学の最先端」
  • Invited
• [Presentation] 水素の量子ゆらぎを考慮した第一原理分子理論の構築と重水素化学への展開 (2021)
  • Author(s): 立川仁典
  • Organizer: 計算で物事を理解する予測する～産業界の実問題に立ち向かうサイエンス～
  • Invited
• [Presentation] Multi-component density functional theory study of H/D isotope effect on phase transition of hydrogen-bonded organic conductor κ-H3(Cat-EDT-TTF)2 (2021)
  • Author(s): Masanori Tachikawa
  • Organizer: MRM2021 Materials Research Meeting
  • Int'l Joint Research
• [Presentation] Quantum Monte Carlo calculation on the effect of molecular vibrations for the positron-binding to polyatomic molecules (2021)
  • Author(s): Masanori Tachikawa
  • Organizer: PACIFICHEM 2021
  • Int'l Joint Research / Invited
• [Presentation] Theoretical study on substituent and solvent effects for nanocube formed with gear-shaped amphiphile molecules (2019)
  • Author(s): Masanori Tachikawa
  • Organizer: THAILAND-JAPAN Symposium in Chemistry
  • Int'l Joint Research / Invited
• [Presentation] Ab initio study of the effect of molecular vibrations on the positron-binding to polyatomic molecules (2019)
  • Author(s): Masanori Tachikawa
  • Organizer: The 23rd International Annual Symposium on Computational Science and Engineering (ANSCSE23)
  • Int'l Joint Research / Invited
• [Presentation] Path integral simulation for accurate calculation of hyperfine coupling constants of hydrogenated and muoniated molecules (2019)
  • Author(s): Masanori Tachikawa
  • Organizer: Isotopes 2019
  • Int'l Joint Research / Invited
• [Presentation] Ab initio study of the effect of molecular vibrations on the positron-binding to polyatomic molecules (2019)
  • Author(s): Masanori Tachikawa
  • Organizer: 15th International Workshop on Slow Positron Beam Techniques & Applications (SLOPOS-15)
  • Int'l Joint Research / Invited
• [Presentation] Path integral simulation for accurate calculation of hyperfine coupling constants of muoniated molecules (2019)
  • Author(s): Masanori Tachikawa
  • Organizer: Ninth Conference of the Asia-Pacific Association of Theoretical and Computational Chemists (APATCC2019),
  • Int'l Joint Research / Invited
• [Remarks] 横浜市立大学量子物理化学研究室（立川・島崎・北グループ）
  • URL: http://www-user.yokohama-cu.ac.jp/~tachi/index.html
• [Remarks] 横浜市立大学量子物理化学研究室（立川・石元・北グループ）
  • URL: http://www-user.yokohama-cu.ac.jp/~tachi/index.html
• [Funded Workshop] 6th Japan-Thai Workshop on Theoretical and Computational Chemistry・横浜（オンライン開催） (2021)