Development of novel simulation methods for excited-state reaction dynamics in condensed phases

• Project/Area Number: 24550022
• Research Category: Grant-in-Aid for Scientific Research (C)
• Allocation Type: Multi-year Fund
• Section: 一般
• Research Field: Physical chemistry
• Research Institution: Kyoto University
• Principal Investigator: YAMAMOTO Takeshi 京都大学, 理学(系)研究科(研究院), 助教 (30397583)
• Project Period (FY): 2012-04-01 – 2015-03-31
• Project Status: Completed (Fiscal Year 2014)
• Budget Amount: ¥5,590,000 (Direct Cost: ¥4,300,000、Indirect Cost: ¥1,290,000); Fiscal Year 2014: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000); Fiscal Year 2013: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000); Fiscal Year 2012: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000)
• Keywords: 溶液反応 / 自由エネルギー / QM/MM / 励起状態 / 統計力学 / 電子状態 / 化学反応 / 溶媒効果 / ダイナミクス

Outline of Final Research Achievements

Excited state dynamics in condensed phases can be studied by QM/MM methods; however, there exist two major problems related to the accuracy of electronic structure theory and a sufficient sampling of system trajectories. In this study we investigated three methods for dealing with this problem: (1) Application of dynamical mean-field method to the solvent dynamics; (2) Approximate way to describe electronic relaxation from excited states based on chain-of-replicas methods; and (3) Efficient QM/MM method based on solute coordinate R and solvent potential V.

Research Products

• [Journal Article] Like-Charge Attraction of Molecular Cations in Water: Subtle Balance between Interionic Interactions and Ionic Solvation Effect (2014)
  • Author(s): Taichi Inagaki, Hiroshi Nakano, Shinji Aono, Takeshi Yamamoto
  • Journal Title: The Journal of Physical Chemistry B Volume: 118 Issue: 20 Pages: 5499-5508
  • DOI: 10.1021/jp501212y
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] Critical Role of Deep Hydrogen Tunneling to Accelerate the Antioxidant Reaction of Ubiquinol and Vitamin E (2014)
  • Author(s): Taichi Inagaki and Takeshi Yamamoto
  • Journal Title: The Journal of Physical Chemistry B Volume: 118 Issue: 4 Pages: 937-950
  • DOI: 10.1021/jp410263f
  • Peer Reviewed
• [Journal Article] Accurate and Efficient Treatment of Continuous Solute Charge Density in the Mean-Field QM/MM Free Energy Calculation (2013)
  • Author(s): H. Nakano, T. Yamamoto
  • Journal Title: Journal of Chemical Theory and Computation Volume: 9 Issue: 1 Pages: 188-203
  • DOI: 10.1021/ct300831t
  • Peer Reviewed
• [Journal Article] Variational calculation of quantum mechanical/molecular mechanical free energy with electronic polarization of solvent (2012)
  • Author(s): H. Nakano, T. Yamamoto
  • Journal Title: The Journal of Chemical Physics Volume: 136 Issue: 13 Pages: 134107-134107
  • DOI: 10.1063/1.3699234
  • NAID: 120005439722
  • Peer Reviewed
• [Journal Article] Including charge penetration effects into the ESP derived partial charge operator (2012)
  • Author(s): H. Nakano, T. Yamamoto
  • Journal Title: Chemical. Physics. Letters Volume: 546 Pages: 80-85
  • DOI: 10.1016/j.cplett.2012.07.046
  • Peer Reviewed
• [Presentation] Supramolecular binding thermodynamics of a gear-shaped nanocube (2014)
  • Author(s): Takeshi Yamamoto, Ryohei Kirihara, Taichi Inagaki, Hirofumi Sato
  • Organizer: Computational Science Workshop 2014
  • Place of Presentation: AIST, Tsukuba
  • Year and Date: 2014-08-20 – 2014-08-22
• [Presentation] トンネル効果と反応物錯体形成が引き起こす抗酸化反応の活性化: ユビキノール-ビタミンE 間の水素移動反応 (2013)
  • Author(s): 稲垣泰一、山本武志
  • Organizer: 第７回分子科学討論会2013京都
  • Place of Presentation: 京都市 京都テルサ
• [Presentation] 電荷密度を用いた平均場 QM/MM 自由エネルギー計算 (2013)
  • Author(s): 中農浩史、山本武志
  • Organizer: 第16回理論化学討論会2013福岡
  • Place of Presentation: 福岡市 健康づくりサポートセンター
• [Presentation] MF-QM/MM法による化学反応の自由エネルギー計算と溶液・酵素反応への応用 (2012)
  • Author(s): 山本武志
  • Organizer: 分子科学討論会
  • Place of Presentation: 東京大学
• [Presentation] QM/MM計算における波動関数の統計揺らぎの効果と平均場近似の妥当性の検証 (2012)
  • Author(s): 中農浩史
  • Organizer: 分子科学討論会
  • Place of Presentation: 東京大学
• [Presentation] 溶液内水素移動反応のトンネリンク効果:ユビキノール-ビタミンEの抗酸化反応 (2012)
  • Author(s): 稲垣泰一
  • Organizer: 分子科学討論会
  • Place of Presentation: 東京大学
• [Presentation] 平均場QM/MM法による溶液・酵素反応の自由エネルギー計算 (2012)
  • Author(s): 中農浩史
  • Organizer: 溶液化学シンポジウム
  • Place of Presentation: 早稲田大学