2022 Fiscal Year Final Research Report
Theoretical elucidation of dynamical solvent effects in controling chemical reactions
| Project/Area Number |
16KT0050
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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 | Shizuoka University |
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Principal Investigator |
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| Co-Investigator(Kenkyū-buntansha) |
山下 雄史 東京大学, 先端科学技術研究センター, 特任准教授 (50615622)
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| Project Period (FY) |
2016-07-19 – 2023-03-31
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| Keywords | 反応動力学 / 機械学習 / エネルギー移動 / 反応性境界 / 相空間構造 / 異性化反応 / 化学物理 / 溶媒効果 |
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| Outline of Final Research Achievements |
Phase space structures in the vicinity of transition state were investigated with the focus on the effects of surrounding molecules. As the target system, the effect of the presence of Ar on the isomerization reaction HCN->CNH was investigated. The potential energy surface function is developed based on ab initio calculations, and phase space structures in the transition state region were extracted through classical trajectory simulations. Subsequently, the reactivity, that is, whether the reaction occurs or not from a given initial condition, was learned as a function of the initial condition. The prediction accuracy was found to be greater than 95 %, indicating that the machine learning captured the features of the phase space that affect the reactivity. Subsequent analyses on the machine learning results revealed the importance of each coordinate in the initial condition.
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| Free Research Field |
理論化学
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| Academic Significance and Societal Importance of the Research Achievements |
化学反応は原子が動くことによって起こるものであり，特に反応途中にある遷移状態とよばれる分割面の付近での原子の動きが，反応の成否を決定するうえで重要である。本研究では，遷移状態付近の原子の動きに対する「溶媒」などの周辺分子の影響を，機械学習を通じて詳細に解析した。それによって，各原子の初期位置および初速度の中で，反応の成否を決定づけるうえで重要度の高い因子と低い因子を判別することを可能にした。この結果は，化学反応に対する基礎科学的知見を推進するとともに，将来的には多様な化学反応の制御につながっていく可能性がある。
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