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Theoretical study on the excited states and emission mechanisms of molecular crystals

Publicly Offered Research

Project AreaSoft Crystals: Science and Photofunctions of Easy-Responsive Systems with Felxibility and Higher-Ordering
Project/Area Number 18H04496
Research Category

Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)

Allocation TypeSingle-year Grants
Research InstitutionHokkaido University

Principal Investigator

岩佐 豪  北海道大学, 理学研究院, 助教 (80596685)

Project Period (FY) 2018-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥4,940,000 (Direct Cost: ¥3,800,000、Indirect Cost: ¥1,140,000)
Fiscal Year 2019: ¥2,470,000 (Direct Cost: ¥1,900,000、Indirect Cost: ¥570,000)
Fiscal Year 2018: ¥2,470,000 (Direct Cost: ¥1,900,000、Indirect Cost: ¥570,000)
Keywords分子結晶 / 分子間相互作用 / 電荷移動励起状態 / 励起状態 / CC2 / DFT-D3
Outline of Annual Research Achievements

分子結晶中の励起状態分子の研究では、分子間相互作用の強さに応じた計算手法が必要である。本研究では、分子間相互作用を無視できる系から二分子にまたがった新たな電子状態を伴う系まで広く対象として、方法論の開発や実験との共同研究を行ってきた。
本年度の成果として、まず3つの異なる置換基を持つホスフィン分子PR1R2R3の励起状態におけるキラル反転(傘反転)の実験を対象に、計算から励起状態によってはほとんどエネルギー障壁が無くなることを示した。また一般性があることも示すために、PH3とPMe3でも同様の振る舞いが見られることを示し論文として報告した。これに加えて、光照射によって発光増強を示す金イソシアニド錯体の結晶構造および光物理特性の解明のために、粉末X線回折パターンから予測された構造に対して、金錯体二分子の励起状態計算を行い、吸収波長の変化をサポートする結果を得た。
一方で、多結晶を示す金錯体の励起状態計算では、ある構造ではAu-Au間にまたがる軌道がLUMOに見られるが、このLUMOに遷移したS1状態での構造最適化を行うと、DFT法では二分子は解離し、DFT-D3法ではπ-π相互作用が強くAu-Au間には結合がない構造が得られた。高精度量子化学計算手法のCC2法を用いたところ、Au-Au間の結合は見られたが、Au-C間の結合も生成した。これらの計算において、実験結果はまだ再現できていない。その原因として、周囲の分子を無視していることが考えられる。計算コストを考えるとDFT-D3法が望ましいが、D3パラメータの金錯体を記述できるようにする必要がある。今後は、CC2計算の結果を参考にD3パラメータを調整し、周囲の分子を古典的に扱い、電荷移動状態も記述可能なLC-DFT-D3/MM法を開発して、多彩な分子間相互作用を持つソフトクリスタルの励起状態の学理を解明していく。

Research Progress Status

令和元年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

令和元年度が最終年度であるため、記入しない。

Report

(2 results)
  • 2019 Annual Research Report
  • 2018 Annual Research Report
  • Research Products

    (18 results)

All 2020 2019 2018

All Journal Article (13 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 13 results,  Open Access: 3 results) Presentation (5 results)

  • [Journal Article] Single-molecule resonance Raman effect in a plasmonic nanocavity2020

    • Author(s)
      Jaculbia Rafael B.、Imada Hiroshi、Miwa Kuniyuki、Iwasa Takeshi、Takenaka Masato、Yang Bo、Kazuma Emiko、Hayazawa Norihiko、Taketsugu Tetsuya、Kim Yousoo
    • Journal Title

      Nature Nanotechnology

      Volume: 15 Issue: 2 Pages: 105-110

    • DOI

      10.1038/s41565-019-0614-8

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Photo‐Induced Pyramidal Inversion Behavior of Phosphines Involved with the Aggregation‐Induced Emission (AIE) Behavior2020

    • Author(s)
      Machida Takashi、Iwasa Takeshi、Taketsugu Tetsuya、Sada Kazuki、Kokado Kenta
    • Journal Title

      Chemistry - A European Journal

      Volume: 26 Issue: 36 Pages: 8028-8034

    • DOI

      10.1002/chem.202000264

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Combined Computational Quantum Chemistry and Classical Electrodynamics Approach for Surface Enhanced Infrared Absorption Spectroscopy2020

    • Author(s)
      M. Takenaka, T. Taketsugu, T. Iwasa
    • Journal Title

      The Journal of Chemical Physics

      Volume: -

    • NAID

      120007029083

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Roles of silver nanoclusters in surface-enhanced Raman spectroscopy2019

    • Author(s)
      T. Tsuneda, T. Iwasa, T. Taketsugu
    • Journal Title

      The Journal of Chemical Physics

      Volume: 151 Issue: 9 Pages: 094102-094102

    • DOI

      10.1063/1.5111944

    • NAID

      120006733158

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] First principles calculations toward understanding SERS of 2,2'-bipyridyl adsorbed on Au, Ag and Au-Ag alloy2019

    • Author(s)
      M. Takenaka, Y. Hashimoto, T. Iwasa, T. Taketsugu, G. Seniutinas, A. Balcytis, S. Juodkazise, Y. Nishijima
    • Journal Title

      Journal of Computational Chemistry

      Volume: 40 Issue: 8 Pages: 925-932

    • DOI

      10.1002/jcc.25603

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Structural and Electronic Properties, Isomerization, and NO Dissociation Reactions on Au, Ag, Cu Clusters2019

    • Author(s)
      Yusuke KONDO, Rina TAKAHARA, Hirono MOHRI, Makito TAKAGI, Satoshi MAEDA, Takeshi IWASA, Tetsuya TAKETSUGU
    • Journal Title

      Journal of Computer Chemistry, Japan

      Volume: 18 Issue: 1 Pages: 64-69

    • DOI

      10.2477/jccj.2018-0044

    • NAID

      130007603140

    • ISSN
      1347-1767, 1347-3824
    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Combined Automated Reaction Pathway Searches and Sparse Modeling Analysis for Catalytic Properties of Lowest Energy Twins of Cu132019

    • Author(s)
      T. Iwasa, T. Sato, M. Takagi, M. Gao, A. Lyalin, M. Kobayashi, K. Shimizu, S. Maeda, T. Taketsugu
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 123 Issue: 1 Pages: 210-217

    • DOI

      10.1021/acs.jpca.8b08868

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Ammonia-rich combustion and ammonia combustive decomposition properties of various supported catalysts2019

    • Author(s)
      S. Hinokuma, K. Araki, T. Iwasa, S. Kiritoshi, Y. Kawabata, T. Taketsugu, and M. Machida
    • Journal Title

      Catalysis Communications

      Volume: 123 Pages: 64-68

    • DOI

      10.1016/j.catcom.2019.02.005

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photoluminescence Properties of [Core+exo]-Type Au6 Clusters: Insights into the Effect of Ligand Environments on the Excitation Dynamics2019

    • Author(s)
      Y. Shichibu, M. Zhang, T. Iwasa, Y. Ono, T. Taketsugu, S. Omagari, T. Nakanishi, Y. Hasegawa, K. Konishi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 123 Issue: 11 Pages: 6934-6939

    • DOI

      10.1021/acs.jpcc.9b01810

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Low-lying Excited States of hqxcH and Zn-hqxc Complex: Toward Understanding Intramolecular Proton Transfer Emission2019

    • Author(s)
      M. Ebina, Y. Kondo, T. Iwasa, T. Taketsugu
    • Journal Title

      Inorganic Chemistry

      Volume: 58 Issue: 7 Pages: 4686-4698

    • DOI

      10.1021/acs.inorgchem.9b00410

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Insights into geometries, stabilities, electronic structures, reactivity descriptors, and magnetic properties of bimetallic NimCun-m (m=1, 2; n=3-13) clusters: Comparison with pure copper clusters2018

    • Author(s)
      Raman K. Singh Takeshi Iwasa Tetsuya Taketsugu
    • Journal Title

      Journal of Computational Chemistry

      Volume: 39 Issue: 23 Pages: 1878-1889

    • DOI

      10.1002/jcc.25361

    • NAID

      120006718708

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Spiral Eu(III) coordination polymers with circularly polarized luminescence2018

    • Author(s)
      Yasuchika Hasegawa, Yui Miura, Yuichi Kitagawa, Satoshi Wada, Takayuki Nakanishi, Koji Fushimi, Tomohiro Seki, Hajime Ito, Takeshi Iwasa, Tetsuya Taketsugu, Masayuki Gon, Kazuo Tanaka, Yoshiki Chujo, Shingo Hattori, Masanobu Karasawa and Kazuyuki Ishii
    • Journal Title

      Chemical Communications

      Volume: 54 Issue: 76 Pages: 10695-10697

    • DOI

      10.1039/c8cc05147j

    • NAID

      120006727594

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Supported binary CuOx catalysts with high activity and thermal stability for the combustion of NH3 as a carbon-free energy source2018

    • Author(s)
      S. Kiritoshi, T. Iwasa, K. Araki, Y. Kawabata, T. Taketsugu, S. Hinokuma, and M. Machida
    • Journal Title

      RSC Advances

      Volume: 8 Issue: 72 Pages: 41491-41498

    • DOI

      10.1039/c8ra07969b

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] 金錯体二量体の励起状態計算:CC2法とDFT-D3法の比較検討2019

    • Author(s)
      岩佐豪、武次徹也
    • Organizer
      第22回理論化学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] DFT-D3 and CC2 study for Pt and Au complexes: Toward understanding of the excited states of Soft Crystals2019

    • Author(s)
      T. Iwasa, M. Miyamoto, T. Taketsugu
    • Organizer
      The 2nd International Symposium on Soft Crystals
    • Related Report
      2019 Annual Research Report
  • [Presentation] 金チオラートクラスターの高位励起状態と発光2018

    • Author(s)
      岩佐豪、蝦名昌徳、原渕祐、武次徹也
    • Organizer
      第30回配位化合物の光化学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 励起プロトン移動由来発光性亜鉛錯体の励起状態と発光機構2018

    • Author(s)
      蝦名昌徳、岩佐豪、武次徹也
    • Organizer
      第30回配位化合物の光化学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 励起プロトン移動由来発光性亜鉛錯体の配位子の発光挙動に関する理論的研究2018

    • Author(s)
      蝦名昌徳、岩佐豪、武次徹也
    • Organizer
      第12回分子科学討論会2018福岡
    • Related Report
      2018 Annual Research Report

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Published: 2018-04-23   Modified: 2021-01-27  

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