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シングレットフィッションにより誘起される非線形光学現象の理論的解明と物質設計

Research Project

Project/Area Number 18J20887
Research Category

Grant-in-Aid for JSPS Fellows

Allocation TypeSingle-year Grants
Section国内
Research Field Physical chemistry
Research InstitutionOsaka University

Principal Investigator

永海 貴識  大阪大学, 基礎工学研究科, 特別研究員(DC1)

Project Period (FY) 2018-04-25 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥3,100,000 (Direct Cost: ¥3,100,000)
Fiscal Year 2020: ¥1,000,000 (Direct Cost: ¥1,000,000)
Fiscal Year 2019: ¥1,000,000 (Direct Cost: ¥1,000,000)
Fiscal Year 2018: ¥1,100,000 (Direct Cost: ¥1,100,000)
Keywordsシングレットフィッション / 一重項分裂 / 非線形光学 / 開殻分子 / 振電相互作用 / 結晶場効果 / 励起子ダイナミクス / 量子マスター方程式 / ジラジカル / 開殻一重項 / 交換積分
Outline of Annual Research Achievements

採用最終年度である本年度はSF-induced-NLO現象のうち、シングレットフィッション(SF)過程に重点を置いて研究を行い、主に(i)新規SF単分子色素の探索、(ii)SFに寄与する振電相互作用の解明、(iii)結晶場効果がSFダイナミクスに及ぼす影響の検討を行った。(i)SF単分子設計の新たな基軸として、従来の開殻性に加え、交換積分の寄与に基づいた分子設計が有効であることを新たに示し、特に小サイズ色素への多重ヘテロ置換によって種々の新規SF色素を見出すことに成功した。(ii)振電相互作用に関しては、前年度の制約つき密度汎関数法に基づく計算法による検討をさらに発展させ、空間密度解析によって振電相互作用を制御する具体的な化学修飾について検討した。(iii)マクロ系の設計で重要となる結晶場効果については、古典分極力場を用いた計算法を導入し、結晶場効果による電荷移動状態の安定化と励起子移動がSF効率に及ぼす影響を、量子マスター方程式および相対緩和因子を用いた解析から解明することに成功した。
以上より、本年度の取り組みによって、従来不完全であったミクロ(単分子)からマクロ(結晶)の空間スケール全体を俯瞰した現象のメカニズム解明と、空間スケール相互のフィードバックに基づく高効率SF物質設計の在り方を初めて示すことに成功している。得られた知見や用いた解析手法は、元の計画にあったSF-induced-NLO現象の解明のみならず、ミクロからマクロに亘る励起状態ダイナミクスやそれに基づく様々な物性発現やその制御にも適用可能であり、今後のSF関連研究の進展にも大きく寄与すると期待される。これらの成果は、国際的な学術雑誌にて複数報告済みである。

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。

Report

(3 results)
  • 2020 Annual Research Report
  • 2019 Annual Research Report
  • 2018 Annual Research Report
  • Research Products

    (28 results)

All 2021 2020 2019 2018 Other

All Int'l Joint Research (1 results) Journal Article (13 results) (of which Int'l Joint Research: 4 results,  Peer Reviewed: 13 results,  Open Access: 2 results) Presentation (14 results) (of which Int'l Joint Research: 7 results)

  • [Int'l Joint Research] ナミュール大学(ベルギー)

    • Related Report
      2018 Annual Research Report
  • [Journal Article] Stabilization of Charge-Transfer States in Pentacene Crystals and Its Role in Singlet Fission2021

    • Author(s)
      Nagami Takanori、Miyamoto Hajime、Sakai Ryota、Nakano Masayoshi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 125 Issue: 4 Pages: 2264-2275

    • DOI

      10.1021/acs.jpcc.0c10029

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Theoretical Study on Singlet Fission in Aromatic Diaza s-Indacene Dimers2021

    • Author(s)
      Nagami Takanori、Sugimori Ryota、Sakai Ryota、Okada Kenji、Nakano Masayoshi
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: - Issue: 16 Pages: 3257-3267

    • DOI

      10.1021/acs.jpca.0c11598

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Molecular Design Principle for Efficient Singlet Fission Based on Diradical Characters and Exchange Integrals: Multiple Heteroatom Substitution Effect on Anthracenes2020

    • Author(s)
      Takanori Nagami, Kenji Okada, Hajime Miyamoto, Wataru Yoshida, Takayoshi Tonami, Masayoshi Nakano
    • Journal Title

      J. Phys. Chem. C

      Volume: 124 Issue: 22 Pages: 11800-11809

    • DOI

      10.1021/acs.jpcc.0c02369

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Theoretical Molecular Design of Phenanthrenes for Singlet Fission by Diazadibora-Substitution2020

    • Author(s)
      Takanori Nagami, Hajime Miyamoto, Wataru Yoshida, Kenji Okada, Takayoshi Tonami, Masayoshi Nakano
    • Journal Title

      J. Phys. Chem. A

      Volume: 124 Issue: 34 Pages: 6778-6789

    • DOI

      10.1021/acs.jpca.0c05359

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Vibronic coupling density analysis and quantum dynamics simulation for singlet fission in pentacene and its halogenated derivatives2020

    • Author(s)
      Nagami Takanori、Tonami Takayoshi、Okada Kenji、Yoshida Wataru、Miyamoto Hajime、Nakano Masayoshi
    • Journal Title

      The Journal of Chemical Physics

      Volume: 153 Issue: 13 Pages: 134302-134302

    • DOI

      10.1063/5.0024746

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Theoretical Study of Non-Markov Effects on Singlet Fission Dynamics of Model Pentacene Dimers Using the Second-Order Time-Convolutionless Quantum Master Equation Method2020

    • Author(s)
      Wataru Yoshida, Kenji Okada, Hajime Miyamoto, Takayoshi Tonami, Takanori Nagami, Masayoshi Nakano
    • Journal Title

      J. Phys. Chem. C

      Volume: 124 Issue: 23 Pages: 12220-12229

    • DOI

      10.1021/acs.jpcc.0c01892

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Quantum design for singlet-fission-induced nonlinear optical systems: Effects of π-conjugation length and molecular packing of butterfly-shaped acenes2020

    • Author(s)
      Tonami Takayoshi、Nagami Takanori、Okada Kenji、Yoshida Wataru、Miyamoto Hajime、Nakano Masayoshi
    • Journal Title

      The Journal of Chemical Physics

      Volume: 153 Issue: 8 Pages: 084304-084304

    • DOI

      10.1063/5.0013985

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Breakdown of the Perturbative Approach to Molecular Packing Dependence of Singlet Fission Rates in Pentacene Dimer Models: A Systematic Comparison with the Quantum Master Equation Approach2019

    • Author(s)
      Okada Kenji、Tonami Takayoshi、Nagami Takanori、Nakano Masayoshi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 123 Issue: 25 Pages: 15403-15411

    • DOI

      10.1021/acs.jpcc.9b01713

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Singlet-Fission-Induced Enhancement of Third-Order Nonlinear Optical Properties of Pentacene Dimers2019

    • Author(s)
      Tonami Takayoshi、Nagami Takanori、Okada Kenji、Yoshida Wataru、Nakano Masayoshi
    • Journal Title

      ACS Omega

      Volume: 4 Issue: 14 Pages: 16181-16190

    • DOI

      10.1021/acsomega.9b02378

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Monte Carlo Wavefunction Approach to Singlet Fission Dynamics of Molecular Aggregates2019

    • Author(s)
      Nakano Masayoshi、Okada Kenji、Nagami Takanori、Tonami Takayoshi、Kishi Ryohei、Kitagawa Yasutaka
    • Journal Title

      Molecules

      Volume: 24 Issue: 3 Pages: 541-541

    • DOI

      10.3390/molecules24030541

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Evaluation of Aromaticity for Open-Shell Singlet Dicyclopenta-Fused Acenes and Polyacenes Based on a Magnetically Induced Current2018

    • Author(s)
      Nagami Takanori、Fujiyoshi Jun-ya、Tonami Takayoshi、Watanabe Ken-ichiro、Yamane Masaki、Okada Kenji、Kishi Ryohei、Nakano Masayoshi、Champagne Benoit、Liegeois Vincent
    • Journal Title

      Chemistry - A European Journal

      Volume: 24 Issue: 51 Pages: 13457-13466

    • DOI

      10.1002/chem.201802696

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Open-Shell Characters, Aromaticities and Third-Order Nonlinear Optical Properties of Carbon Nanobelts Composed of Five- and Six-Membered Rings2018

    • Author(s)
      Yamane Masaki、Kishi Ryohei、Tonami Takayoshi、Okada Kenji、Nagami Takanori、Kitagawa Yasutaka、Nakano Masayoshi
    • Journal Title

      Asian Journal of Organic Chemistry

      Volume: 7 Issue: 11 Pages: 2320-2329

    • DOI

      10.1002/ajoc.201800390

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Quantum Master Equation Approach to Singlet Fission Dynamics in Pentacene Linear Aggregate Models: Size Dependences of Excitonic Coupling Effects2018

    • Author(s)
      Nakano Masayoshi、Nagami Takanori、Tonami Takayoshi、Okada Kenji、Ito Soichi、Kishi Ryohei、Kitagawa Yasutaka、Kubo Takashi
    • Journal Title

      Journal of Computational Chemistry

      Volume: 40 Issue: 1 Pages: 89-104

    • DOI

      10.1002/jcc.25539

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Presentation] ジラジカル因子と交換積分に基づく新奇シングレットフィッション分子の設計原理:小サイズ色素への多重ヘテロ原子置換効果2020

    • Author(s)
      永海貴識、當波孝凱、岡田健治、吉田航、宮本孟、杉森良太、中野雅由
    • Organizer
      分子科学オンライン討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 高効率シングレットフィッションに向けた振電相互作用設計に関する理論研究2020

    • Author(s)
      永海貴識、當波孝凱、岡田健治、吉田航、宮本孟、中野雅由
    • Organizer
      第17回京都大学福井謙一記念研究センターシンポジウム
    • Related Report
      2019 Annual Research Report
  • [Presentation] Theoretical study on the vibronic coupling in singlet fission for pentacene dimer models2020

    • Author(s)
      Takanori Nagami, Takayoshi Tonami, Kenji Okada, Wataru Yoshida, Hajime Miyamoto, Masayoshi Nakano
    • Organizer
      日本化学会第100春季年会
    • Related Report
      2019 Annual Research Report
  • [Presentation] シングレットフィッションにおける振電相互作用設計のconstrained-DFT法による理論研究2019

    • Author(s)
      永海貴識、當波孝凱、岡田健治、吉田航、宮本孟、中野雅由
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] VIbronic Coupling Density Analysis for Singlet Fission in Terrylene Dimers2019

    • Author(s)
      Takanori Nagami, Takayoshi Tonami, Kenji Okada, Masayoshi Nakano
    • Organizer
      7th International Symposium on π-System Figuration
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Theoretical Study on the Effect of Vibronic Couplings in Singlet Fission of Terrylene Dimers2019

    • Author(s)
      Takanori Nagami, Takayoshi Tonami, Kenji Okada, Masayoshi Nakano
    • Organizer
      10th International Conference on Materials for Advanced Technologies
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Theoretical Study on the Aromaticity of Open-Shell Singlet Molecules by the GIMIC Method2019

    • Author(s)
      Takanori Nagami, Takayoshi Tonami, Kenji Okada, Masayoshi Nakano
    • Organizer
      10th International Conference on Materials for Advanced Technologies
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Theoretical Study on Singlet Fission in Pentacene Dimer Model Based on Vibronic Coupling and its Density Analysis2019

    • Author(s)
      Takanori Nagami, Takayoshi Tonami, Kenji Okada, Wataru Yoshida, Hajime Miyamoto, Masayoshi Nakano
    • Organizer
      Final International Symposium on Photosynergetics
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] テリレンのシングレットフィッションにおける振電相互作用に関する理論研究2019

    • Author(s)
      永海 貴識、伊藤 聡一、當波 孝凱、岡田 健治、中野 雅由
    • Organizer
      第15回京都大学福井謙一記念研究センターシンポジウム
    • Related Report
      2018 Annual Research Report
  • [Presentation] Vibronic Coupling Density Analysis for Singlet Fission in Terrylene Dimers2019

    • Author(s)
      Takanori Nagami、Takayoshi Tonami、Kenji Okada、Masayoshi Nakano
    • Organizer
      7th International Symposium on π-System Figuration
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 磁場誘導電流の量子化学計算に基づいた開殻一重項分子における芳香族性の検討2018

    • Author(s)
      永海 貴識、當波 孝凱、中野 雅由、Benoit Champagne、Vincent Liegeois
    • Organizer
      第21回理論化学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] テリレンの高効率シングレットフィッションを目指した振電相互作用設計に関する理論研究2018

    • Author(s)
      永海 貴識、伊藤 聡一、當波 孝凱、岡田 健治、中野 雅由
    • Organizer
      第12回分子科学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] GIMIC approach to the evaluation of aromaticity of open-shell singlet polycyclic hydrocarbons2018

    • Author(s)
      Takanori Nagami、Takayoshi Tonami、Masayoshi Nakano、Benoit Champagne、Vincent Liegeois
    • Organizer
      Theoretical Studies of Magnetic Systems: Methodological Developments and Applications. (Satellite Symposium of ICQC 2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Density analysis of vibronic couplings toward efficient singlet fission in terrylene derivatives2018

    • Author(s)
      Takanori Nagami、Soichi Ito、Takayoshi Tonami、Kenji Okada、Masayoshi Nakano
    • Organizer
      16th International Congress of Quantum Chemistry (ICQC2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research

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Published: 2018-05-01   Modified: 2024-03-26  

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