Theoretical study of reaction path bifurcation mapped on the global reaction route map
| Project/Area Number |
16KT0047
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| Research Category |
Grant-in-Aid for Scientific Research (B)
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| Allocation Type | Multi-year Fund |
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| Section | 特設分野 |
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| Research Field |
Transition State Control
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| Research Institution | Hokkaido University |
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Principal Investigator |
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| Research Collaborator |
MAEDA Satoshi
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| Project Period (FY) |
2016-07-19 – 2019-03-31
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| Project Status |
Completed (Fiscal Year 2018)
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| Budget Amount *help |
¥18,590,000 (Direct Cost: ¥14,300,000、Indirect Cost: ¥4,290,000)
Fiscal Year 2018: ¥5,590,000 (Direct Cost: ¥4,300,000、Indirect Cost: ¥1,290,000)
Fiscal Year 2017: ¥5,590,000 (Direct Cost: ¥4,300,000、Indirect Cost: ¥1,290,000)
Fiscal Year 2016: ¥7,410,000 (Direct Cost: ¥5,700,000、Indirect Cost: ¥1,710,000)
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| Keywords | 反応経路分岐 / 反応経路地図 / 谷-尾根遷移 / 固有反応座標 / ポテンシャル曲面 / 第一原理分子動力学 / 金クラスター / 励起状態 / 遷移状態 / スチルベン誘導体 / 古典的多次元尺度構成法 / AIMD / IRC / 谷尾根遷移 |
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| Outline of Final Research Achievements |
The intrinsic reaction coordinate (IRC) is defined as a static reaction path for an elementary reaction. In some case, however, the potential curvature in the direction orthogonal to the reaction path changes from positive to negative, and the reaction path bifurcation occurs. In this project, a global reaction path map is generated for a small gold cluster, as an example, by anharmonic downward distortion following method and IRC calculation, and the condition and frequency at which a reaction path bifurcation occurs are investigated. It is shown that there always exists a transition state in the region close to the valley-ridge transition point. The dynamics effect and branching ratio are further analyzed by AIMD simulations, which leads to a proposal of a dynamical reaction picture.
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| Academic Significance and Societal Importance of the Research Achievements |
原子・分子の世界を支配する原理である量子力学を基盤とする量子化学計算は計算機の進展とともに大いに発展し、化学反応の研究では量子化学計算に基づく固有反応座標を用いるのがルーチンとなり、さらに反応経路自動探索法の出現により網羅的にIRCを求める計算が可能となって、化学反応研究が多いに進展した。しかしポテンシャル曲面の情報のみで決められる静的反応経路は、経路分岐や経路の曲がりなどによる動的効果により破たんする可能性がある。本研究では、反応経路自動探索法と第一原理分子動力学計算を駆使することにより、静的反応描像を超えた動的反応描像の構築を目指すものであり、次世代化学反応理論への道を拓くものである。
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Report
(4 results)
Research Products
(30 results)
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[Journal Article] Multi-Step Intersystem Crossing Pathways in Cinnamate-Based UV-B Sunscreens2016
Author(s)
K. Yamazaki, Y. Miyazaki, Y. Harabuchi, T. Taketsugu, S. Maeda, Y. Inokuchi, S.-N. Kinoshita, M. Sumida, Y. Onitsuka, H. Kohguchi, M. Ehara, and T. Ebata
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Journal Title
J. Phys. Chem. Lett.
Volume: 7
Issue: 19
Pages: 4001-4007
DOI
Related Report
Peer Reviewed
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[Presentation] 反応経路分岐の理論化学2016
Author(s)
武次徹也
Organizer
2016年有機反応機構研究会
Place of Presentation
長崎県工業技術センター（長崎県・大村市）
Year and Date
2016-09-05
Related Report
Invited
