Development of multicomponent molecular theories 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: 21H00026
• 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(八景キャンパス), 教授 (00267410)
• Project Period (FY): 2021-04-01 – 2023-03-31
• Project Status: Completed (Fiscal Year 2022)
• Budget Amount: ¥3,640,000 (Direct Cost: ¥2,800,000、Indirect Cost: ¥840,000); Fiscal Year 2022: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000); Fiscal Year 2021: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
• 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、申請者が前回の公募研究で得られた成果をもとに、領域内でのさらなる共同研究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(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。その中でも特に本年度は、LBHBに起因する、金属表面における水素吸着の安定性や量子論的な吸着反応経路の解析を行う。

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した。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。また、実験研究者との密な議論に基づいた高次水素機能の発現機構解明・予測、を行った。具体的には、公募研究B02の加藤先生が中心となり、計画研究A03-2の森先生と計画研究A04の吉信先生と共に、水素ー電子カップリング系2分子膜を「新発想」素子として開発する際に、理論計算の立場で共同研究を実施した。また、公募研究B02の川脇先生らの合成されたAu包接Ni多核錯体の理論計算を実施した。
なお、このような理論計算と実験科学との協奏により、2022年度第9回HPCI利用研究課題優秀成果賞を受賞した。

Research Progress Status

令和4年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

令和4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] Theoretical investigations of positron affinities and their structure-dependent properties of carbon dioxide clusters (CO2)n(n=1~5) (2023)
  • Author(s): Miku Furushima, Makito Takagi, Daisuke Yoshida, Yukiumi Kita, Tomomi Shimazaki and Masanori Tachikawa
  • Journal Title: Physical Chemistry Chemical Physics Volume: 25 Issue: 1 Pages: 625-632
  • DOI: 10.1039/d2cp03788b
  • Peer Reviewed
• [Journal Article] Improved activity for the oxygen evolution reaction using a tiara-like thiolate-protected nickel nanocluster (2023)
  • Author(s): Funaki Sota、Kawawaki Tokuhisa、Okada Tomoshige、Takemae Kana、Hossain Sakiat、Niihori Yoshiki、Naito Takumi、Takagi Makito、Shimazaki Tomomi、Kikkawa Soichi、Yamazoe Seiji、Tachikawa Masanori、Negishi Yuichi
  • Journal Title: Nanoscale Volume: 15 Issue: 11 Pages: 5201-5208
  • DOI: 10.1039/d2nr06952k
  • Peer Reviewed / Open Access
• [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] Ambipolar to unipolar irreversible switching in nanosheet transistors: the role of ferrocene in fullerene/ferrocene nanosheets (2022)
  • Author(s): Mahdaoui Dorra、Hirata Chika、Nagaoka Kahori、Miyazawa Kun’ichi、Fujii Kazuko、Ando Toshihiro、Abderrabba Manef、Ito Osamu、Takagi Makito、Ishimoto Takayoshi、Tachikawa Masanori、Yagyu Shinjiro、Liu Yubin、Nakajima Yoshiyuki、Nemoto Yoshihiro、Tsukagoshi Kazuhito、Wakahara Takatsugu
  • Journal Title: Journal of Materials Chemistry C Volume: 10 Issue: 10 Pages: 3770-3774
  • DOI: 10.1039/d1tc05545c
  • Peer Reviewed / Int'l Joint Research
• [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 Isotope and Homologue Effects on Nuclear Magnetic Shielding in Water and Hydrogen Sulfide Molecules (2022)
  • Author(s): Ishii Kiriko、Shimazaki Tomomi、Tachikawa Masanori、Kita Yukiumi
  • Journal Title: Chemistry Letters Volume: 51 Issue: 3 Pages: 342-344
  • DOI: 10.1246/cl.210760
  • Peer Reviewed
• [Journal Article] Collaborative Approach between Explainable Artificial Intelligence and Simplified Chemical Interactions to Explore Active Ligands for Cyclin-Dependent Kinase 2 (2022)
  • Author(s): Shimazaki Tomomi、Tachikawa Masanori
  • Journal Title: ACS Omega Volume: 7 Issue: 12 Pages: 10372-10381
  • DOI: 10.1021/acsomega.1c06976
  • Peer Reviewed / Open Access
• [Journal Article] Low-Barrier Hydrogen Bond in Fujikurin A?D: A Computational Study (2022)
  • Author(s): Tanaka Hikaru、Kuwahata Kazuaki、Tachikawa Masanori、Udagawa Taro
  • Journal Title: ACS Omega Volume: 7 Issue: 16 Pages: 14244-14251
  • DOI: 10.1021/acsomega.2c00857
  • Peer Reviewed / Open Access
• [Journal Article] Nuclear quantum effect and H/D isotope effect in excited state intramolecular proton transfer and electron‐induced intramolecular proton transfer reactions in 8‐hydroxyquinoline (2022)
  • Author(s): Udagawa Taro、Hattori Ikumi、Kanematsu Yusuke、Ishimoto Takayoshi、Tachikawa Masanori
  • Journal Title: International Journal of Quantum Chemistry Volume: 122 Issue: 19
  • DOI: 10.1002/qua.26962
  • Peer Reviewed
• [Journal Article] Fullerene C70 porphyrin hybrid nanoarchitectures: single-cocrystal nanoribbons with ambipolar charge transport properties (2022)
  • Author(s): Wakahara Takatsugu、Nagaoka Kahori、Hirata Chika、Miyazawa Kun'ichi、Fujii Kazuko、Matsushita Yoshitaka、Ito Osamu、Takagi Makito、Shimazaki Tomomi、Tachikawa Masanori、Wada Yoshiki、Yagyu Shinjiro、Liu Yubin、Nakajima Yoshiyuki、Tsukagoshi Kazuhito
  • Journal Title: RSC Advances Volume: 12 Issue: 30 Pages: 19548-19553
  • DOI: 10.1039/d2ra02669d
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] A path integral molecular dynamics study on the NH₄⁺ rotation in NH₄⁺?XH₂ (X = Be or Mg) dihydrogen bond systems (2022)
  • Author(s): Udagawa Taro、Kinoshita Amane、Kuwahata Kazuaki、Tachikawa Masanori
  • Journal Title: Physical Chemistry Chemical Physics Volume: 24 Issue: 28 Pages: 17295-17302
  • DOI: 10.1039/d2cp01999j
  • Peer Reviewed
• [Journal Article] Theoretical study of the effect of nonlocal short-range exchange on calculations of molecular excitation energies in the dielectric screened-exchange method (2022)
  • Author(s): Shimazaki Tomomi、Tachikawa Masanori
  • Journal Title: Chemical Physics Letters Volume: 802 Pages: 139740-139740
  • DOI: 10.1016/j.cplett.2022.139740
  • Peer Reviewed
• [Journal Article] A comprehensive theoretical study of positron binding and annihilation properties of hydrogen bonded binary molecular clusters (2022)
  • Author(s): Daisuke Yoshida, Yukiumi Kita, Tomomi Shimazaki, Masanori Tachikawa
  • Journal Title: Physical Chemistry Chemical Physics Volume: 24(43) Issue: 43 Pages: 26898-26907
  • DOI: 10.1039/d2cp03813g
  • Peer Reviewed
• [Journal Article] Decomposition analysis on the excitation behaviors of thiazolothiazole (TTz)-based dyes <i>via</i> the time-dependent dielectric density functional theory approach (2022)
  • Author(s): Naito Takumi、Kita Yukiumi、Shimazaki Tomomi、Tachikawa Masanori
  • Journal Title: RSC Advances Volume: 12 Issue: 53 Pages: 34685-34693
  • DOI: 10.1039/d2ra06454e
  • Peer Reviewed / Open Access
• [Journal Article] Molecular Dynamics Study on the Structure-Property Relationship of Self-Assembled Gear-Shaped Amphiphile Molecules with/without Methyl Groups (2022)
  • Author(s): Murata Moe、Koide Takuya、Kobayashi Osamu、Hiraoka Shuichi、Shimazaki Tomomi、Tachikawa Masanori
  • Journal Title: The Journal of Physical Chemistry B Volume: 127 Issue: 1 Pages: 328-334
  • DOI: 10.1021/acs.jpcb.2c07444
  • 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
• [Presentation] Quantum Multi-Component Molecular Theory for H-Bonded System and its H/D Isotope Effect (2023)
  • Author(s): Masanori Tachikawa
  • Organizer: J-PARC Workshop 2022, Deuterium Science to Entering a New Phase
  • Int'l Joint Research / Invited
• [Presentation] Path integral simulation for H/D isotope effect in protonated/deuterated aqueous solution (2023)
  • Author(s): Masanori Tachikawa
  • Organizer: Asia Pacific Conference of Theoretical and Computational Chemistry (APATCC-10)
  • Int'l Joint Research / Invited
• [Presentation] Theoretical study on positron binding to atomic anion dimers: using first-principles Quantum Monte Carlo (2022)
  • Author(s): Masanori Tachikawa
  • Organizer: 19th International Conference on Positron Annihilation (ICPA19)
  • Int'l Joint Research / Invited
• [Presentation] Positron Binding in Molecules (2022)
  • Author(s): Masanori Tachikawa
  • Organizer: 75th Annual Gaseous Electronics Conference (GEC2022)
  • Int'l Joint Research / Invited
• [Presentation] Theoretical study on positron binding to atomic anion dimers: using first-principles Quantum Monte Carlo (2022)
  • Author(s): Masanori Tachikawa
  • Organizer: 第２４回理論化学討論会
• [Presentation] Muon and Positron Binding to Molecules (2022)
  • Author(s): Masanori Tachikawa
  • Organizer: 7th International Symposium of Quantum Beam Science
  • Int'l Joint Research / Invited
• [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] 7th Japan-Thai workshop on Theoretical and Computational Chemistry 2022, Yokohama (2022)
• [Funded Workshop] 6th Japan-Thai Workshop on Theoretical and Computational Chemistry・横浜（オンライン開催） (2021)