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

2020 Fiscal Year Annual Research Report

• Project Area: HYDROGENOMICS: Creation of Innovative Materials, Devices, and Reaction Processes using Higher-Order Hydrogen Functions
• Project/Area Number: 19H05063
• 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
• 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 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)
  • Country Name: THAILAND
  • Counterpart Institution: チェンマイ大学/ウボンラチャタニ大学
• [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 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 Pages: 12814-1～12814-5
  • 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 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 Pages: 1954～1962
  • DOI: 10.1246/bcsj.20210083
  • 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 Pages: 21512～21520
  • DOI: 10.1039/D1CP02808A
• [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 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 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 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 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): Iida Ryusei、Suzuki Haruya、Takayanagi Toshiyuki、Tachikawa Masanori
  • Journal Title: Physical Review A Volume: 104 Pages: 62807-1～62807-9
  • 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 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 Pages: 745～748
  • DOI: 10.1246/cl.200198
  • 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 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): Sugiura Yutaro、Suzuki Haruya、Otomo Takuma、Miyazaki Takaaki、Takayanagi Toshiyuki、Tachikawa Masanori
  • Journal Title: Journal of Computational Chemistry Volume: 41 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): Sakagami Hiroki、Tachikawa Masanori、Ishimoto Takayoshi
  • Journal Title: International Journal of Quantum Chemistry Volume: 120 Pages: 26275-1～26275-5
  • 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 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): Sugiura Yutaro、Takayanagi Toshiyuki、Tachikawa Masanori
  • Journal Title: International Journal of Quantum Chemistry Volume: 120 Pages: 26376-1～26376-5
  • 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): Suzuki Haruya、Otomo Takuma、Iida Ryusei、Sugiura Yutaro、Takayanagi Toshiyuki、Tachikawa Masanori
  • Journal Title: Physical Review A Volume: 102 Pages: 52830-1～52830-9
  • DOI: 10.1103/PhysRevA.102.052830
  • Peer Reviewed
• [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 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 Pages: 1558～1563
  • DOI: 10.1246/bcsj.20200120
  • 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
• [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
• [Funded Workshop] 6th Japan-Thai Workshop on Theoretical and Computational Chemistry・横浜（オンライン開催） (2021)