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Theory of chemical binding in beyond-Born-Oppenheimer chemistry and its applications to complex molecular systems

Research Project

Project/Area Number 20H00373
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Review Section Medium-sized Section 32:Physical chemistry, functional solid state chemistry, and related fields
Research InstitutionKyoto University

Principal Investigator

Takatsuka Kazuo  京都大学, 福井謙一記念研究センター, 研究員 (70154797)

Project Period (FY) 2020-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥45,110,000 (Direct Cost: ¥34,700,000、Indirect Cost: ¥10,410,000)
Fiscal Year 2023: ¥4,810,000 (Direct Cost: ¥3,700,000、Indirect Cost: ¥1,110,000)
Fiscal Year 2022: ¥11,830,000 (Direct Cost: ¥9,100,000、Indirect Cost: ¥2,730,000)
Fiscal Year 2021: ¥14,430,000 (Direct Cost: ¥11,100,000、Indirect Cost: ¥3,330,000)
Fiscal Year 2020: ¥14,040,000 (Direct Cost: ¥10,800,000、Indirect Cost: ¥3,240,000)
Keywords実時間電子ダイナミクス / 電子・スピン流化学 / 非断熱遷移動力学 / 励起状態動力学 / 超高速化学反応 / 化学結合論 / 化学反応理論 / 一般化学結合論 / 一般化学反応理論 / 非断熱電子動力学 / 化学動力学 / 理論化学 / 擬縮重電子状態理論 / クラスタ―化学 / 電子動力学 / 非断熱遷移 / 高擬縮重系 / 反応場 / 電子ダイナミクス / 励起状態化学 / 化学反応論 / レーザー化学 / 電子移動 / プロトン移動
Outline of Research at the Start

新しい化学領域「超ボルン・オッペンハイマー化学」、あるいは「非断熱電子動力学理論」で支配される領域の基礎理論を定式化し、原子核の動きと同期して電子波動関数が実時間変動する様子を直接観る方法論の開拓と応用を行う。これにより、従来の化学理論では得られない化学反応への制御能力や複雑な現象の定性的な予言能力が獲得できる。本課題研究では、以下の2項目に取り組む:動的電子化学反応学の核心となる特徴的な化学結合と化学反応の本質として
項目1 電子状態がびっしり詰まった擬縮重系の化学結合とその反応
さらに、その複雑分子系への新展開として
項目2 複雑分子場中での非断熱電子動力学および励起状態化学のための方法論と応用

Outline of Final Research Achievements

We have studied a new class of chemical dynamics to be found in molecular electronic excited states embedded in densely quasi-degenerate state manifolds, in which a huge fluctuation is induced due to persisting multidimensional nonadiabatic transitions among the states. The relevant phenomena can result in intramolecular energy redistribution, which we call intramolecular nonadiabatic electronic-energy redistribution. Despite the huge fluctuation, strong chemical bonding coexists to assist the molecules to survive. Such complex electronic excited states are found in, for example, boron and carbon clusters. Those excited states have been analyzed with our developed energy natural orbitals (ENO). It turns out that ENO energy spectra are composed of four robust layers of different physical natures. In the layer structure, the physical origin of the robust chemical bonds has been identified. We also have found novel electronic-state quantum chaos behind the fluctuation.

Academic Significance and Societal Importance of the Research Achievements

本研究は、分子の電子状態理論(いわゆる量子化学)の新しい領域を開拓し、将来発展するであろう非断熱電子動力学理論の礎を構築するものである。特に、原子核と電子の多次元多状態非断相互作用、アト秒レベルの実時間電子流・電子エネルギー流・スピン流の実時間追跡、などを解析可能とし、従来の理論的枠組みの中でも有用な手法として応用可能な高励起状態化学の解析手法、などを提案している。

Report

(6 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • 2020 Comments on the Screening Results   Annual Research Report
  • Research Products

    (29 results)

All 2024 2023 2022 2021 Other

All Journal Article (16 results) (of which Peer Reviewed: 11 results,  Open Access: 10 results) Presentation (12 results) (of which Int'l Joint Research: 6 results,  Invited: 6 results) Remarks (1 results)

  • [Journal Article] Geometrical decomposition of nonadiabatic interactions to collective coordinates in many-dimensional and many-state mixed fast?slow dynamics2024

    • Author(s)
      Takatsuka Kazuo
    • Journal Title

      The Journal of Chemical Physics

      Volume: 160 Issue: 4 Pages: 044112-044112

    • DOI

      10.1063/5.0186816

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Sonification of molecular electronic energy density and its dynamics2024

    • Author(s)
      Arasaki Yasuki、Takatsuka Kazuo
    • Journal Title

      RSC Advances

      Volume: 14 Issue: 13 Pages: 9099-9108

    • DOI

      10.1039/d4ra00999a

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Quantum Chaos in the Dynamics of Molecules2023

    • Author(s)
      Takatsuka Kazuo
    • Journal Title

      Entropy

      Volume: 25 Issue: 1 Pages: 63-63

    • DOI

      10.3390/e25010063

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Electronic-state chaos, intramolecular electronic energy redistribution, and chemical bonding in persisting multidimensional nonadiabatic systems2023

    • Author(s)
      Takatsuka Kazuo、Arasaki Yasuki
    • Journal Title

      The Journal of Chemical Physics

      Volume: 159 Issue: 7 Pages: 074110-074110

    • DOI

      10.1063/5.0159178

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Schr?dinger dynamics in length-scale hierarchy: from spatial rescaling to Huygens-like proliferation of Gaussian wavepackets2023

    • Author(s)
      Takatsuka Kazuo
    • Journal Title

      Journal of Physics A: Mathematical and Theoretical

      Volume: 56 Issue: 44 Pages: 445302-445302

    • DOI

      10.1088/1751-8121/acfe63

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Energy natural orbital characterization of nonadiabatic electron wavepackets in the densely quasi-degenerate electronic state manifold2023

    • Author(s)
      Arasaki Yasuki、Takatsuka Kazuo
    • Journal Title

      The Journal of Chemical Physics

      Volume: 158 Issue: 11 Pages: 114102-114102

    • DOI

      10.1063/5.0139288

    • Related Report
      2022 Annual Research Report
  • [Journal Article] Spin current in the early stage of radical reactions and its mechanisms2023

    • Author(s)
      Hanasaki Kota、Takatsuka Kazuo
    • Journal Title

      The Journal of Chemical Physics

      Volume: 159 Issue: 14 Pages: 144111-144111

    • DOI

      10.1063/5.0169281

    • Related Report
      2022 Annual Research Report
  • [Journal Article] Spin current in chemical reactions2022

    • Author(s)
      Hanasaki Kota、Takatsuka Kazuo
    • Journal Title

      Chemical Physics Letters

      Volume: 793 Pages: 139462-139462

    • DOI

      10.1016/j.cplett.2022.139462

    • Related Report
      2022 Annual Research Report 2021 Annual Research Report
  • [Journal Article] Nature of chemical bond and potential barrier in an invariant energy-orbital picture2022

    • Author(s)
      Arasaki Yasuki、Takatsuka Kazuo
    • Journal Title

      The Journal of Chemical Physics

      Volume: 156 Issue: 23 Pages: 234102-234102

    • DOI

      10.1063/5.0088340

    • Related Report
      2022 Annual Research Report
  • [Journal Article] Real-time electronic energy current and quantum energy flux in molecules2022

    • Author(s)
      Takatsuka Kazuo、Arasaki Yasuki
    • Journal Title

      The Journal of Chemical Physics

      Volume: 157 Issue: 24 Pages: 244108-244108

    • DOI

      10.1063/5.0131200

    • Related Report
      2022 Annual Research Report
  • [Journal Article] Suppression of charge recombination by auxiliary atoms in photoinduced charge separation dynamics with Mn oxides: A theoretical study2022

    • Author(s)
      Y. Ohnishi, K Yamamoto, and K. Takatsuka
    • Journal Title

      Molecules

      Volume: 27 Issue: 3 Pages: 755-755

    • DOI

      10.3390/molecules27030755

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Electron dynamics in molecular elementary processes and chemical reactions2021

    • Author(s)
      Kazuo Takatsuka
    • Journal Title

      Bull. Chem. Soc. Jpn

      Volume: 94 Issue: 4 Pages: 1421-1477

    • DOI

      10.1246/bcsj.20200388

    • NAID

      130008037365

    • Related Report
      2021 Annual Research Report 2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] An orbital picture extracted from correlated electronic wavefunctions for symmetry-forbidden and nonadiabatic chemical reactions: 70 years of Fukui frontier orbital theory and beyond.2021

    • Author(s)
      Kazuo Takatsuka and Yasuki Arasaki
    • Journal Title

      J. Chem. Phys.

      Volume: 155 Issue: 6

    • DOI

      10.1063/5.0059370

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Time-dependent variational dynamics for nonadiabatically coupled nuclear and electronic quantum wavepackets in molecules2021

    • Author(s)
      Kazuo Takatsuka
    • Journal Title

      Eur. Phys. J. D

      Volume: 75 Issue: 9

    • DOI

      10.1140/epjd/s10053-021-00263-9

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Energy Natural Orbitals2021

    • Author(s)
      Kazuo Takatsuka and Yasuki Arasaki
    • Journal Title

      J. Chem. Phys.

      Volume: 154 Issue: 9 Pages: 094103-094103

    • DOI

      10.1063/5.0034810

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] On the molecular electronic flux: Roles of nonadiabaticity and violation of conservation2021

    • Author(s)
      Kota Hanasaki and Kazuo Takatsuka
    • Journal Title

      J. Chem. Phys.

      Volume: - Issue: 16

    • DOI

      10.1063/5.0049821

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] Nature of Chemical Bonds in Excited States2023

    • Author(s)
      Kazuo Takatsuka
    • Organizer
      APATCC-10
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Persisting multiple multi-dimensional nonadiabatic interactions in densely quasi-degenerate excited states2023

    • Author(s)
      Kazuo Takatsuka
    • Organizer
      TACC2023
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] ラジカル反応における電子ダイナミクスと スピンフラックス2023

    • Author(s)
      花崎 浩太、高塚 和夫
    • Organizer
      理論化学討論会2023
    • Related Report
      2023 Annual Research Report
  • [Presentation] 励起状態の化学結合論2023

    • Author(s)
      高塚和夫、新崎康樹
    • Organizer
      理論化学討論会2023
    • Related Report
      2023 Annual Research Report
  • [Presentation] 励起状態ボロンクラスターの巨大電子揺らぎと化学結合2023

    • Author(s)
      高塚和夫、新崎康樹
    • Organizer
      分子科学討論会2023
    • Related Report
      2023 Annual Research Report
  • [Presentation] An invariant energy-orbital theory for the nature of chemical bonds and transition states2022

    • Author(s)
      Kazuo Takatsuka
    • Organizer
      Theoretical Chemistry Meeting: Structure and Dynamics (TCMSD-2022)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] フロンティア軌道理論の70年: 電子相関と非断熱相互作用の下の反応論へ2022

    • Author(s)
      高塚和夫,新崎康樹
    • Organizer
      理論化学討論会(2022)
    • Related Report
      2022 Annual Research Report
  • [Presentation] 電子フラックスと非断熱電子動力学2022

    • Author(s)
      花崎 浩太、高塚 和夫
    • Organizer
      分子科学討論会(2022)
    • Related Report
      2022 Annual Research Report
  • [Presentation] From energy-domain to time-domain in quantum chemistry: Nonadiabatic electron dynamics2021

    • Author(s)
      Kazuo Takatsuka
    • Organizer
      Fall 2021National ACS meeting
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Nonadiabatic dynamics and quantum chemistry2021

    • Author(s)
      Fall 2021National ACS meeting (August 22-26, 2021) Symposium “Prominent ideas in quantum chemistry”, online Kazuo Takatsuka
    • Organizer
      Theoretical Chemistry Symposium, India
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Real-time electron dynamics in molecular charge separations2021

    • Author(s)
      Kazuo Takatsuka
    • Organizer
      The 58 Annual Convention of Chemists (Indian Chemical Society)
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] フロンティア軌道理論の70年: 電子相関と非断熱相互作用の下の反応論へ2021

    • Author(s)
      高塚和夫・新崎康樹
    • Organizer
      理論化学討論会
    • Related Report
      2021 Annual Research Report 2020 Annual Research Report
  • [Remarks] 高塚研究室

    • URL

      https://mns2.fukui.kyoto-u.ac.jp/

    • Related Report
      2020 Annual Research Report

URL: 

Published: 2020-04-28   Modified: 2025-01-30  

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