2024-02-15 ミュンヘン大学(LMU)
◆この新しいハイパーリアクターは、緩和されたポテンシャルエネルギー曲面上での化学空間の探索と分子系の周期的収縮を組み合わせることで、穏やかな条件下で複雑な反応ネットワークの研究を可能にする。これにより、新しい計算可能性に関する初期の洞察が得られ、ほかにも新しい高速な量子化学手法と組み合わされることで、広範な化学的および生化学的合成経路の研究に新たな展望が開かれる。
<関連情報>
- https://www.lmu.de/en/newsroom/news-overview/news/theoretical-chemistry-simulation-of-molecular-origins-of-life.html
- https://pubs.acs.org/doi/10.1021/acscentsci.3c01403
Ab Initioハイパーリアクター・ダイナミクスを用いた化学空間の探索 Exploring Chemical Space Using Ab Initio Hyperreactor Dynamics
Alexandra Stan-Bernhardt, Liubov Glinkina, Andreas Hulm, and Christian Ochsenfeld
ACS Central Science Published:January 30, 2024
DOI:https://doi.org/10.1021/acscentsci.3c01403
Abstract
In recent years, first-principles exploration of chemical reaction space has provided valuable insights into intricate reaction networks. Here, we introduce ab initio hyperreactor dynamics, which enables rapid screening of the accessible chemical space from a given set of initial molecular species, predicting new synthetic routes that can potentially guide subsequent experimental studies. For this purpose, different hyperdynamics derived bias potentials are applied along with pressure-inducing spherical confinement of the molecular system in ab initio molecular dynamics simulations to efficiently enhance reactivity under mild conditions. To showcase the advantages and flexibility of the hyperreactor approach, we present a systematic study of the method’s parameters on a HCN toy model and apply it to a recently introduced experimental model for the prebiotic formation of glycinal and acetamide in interstellar ices, which yields results in line with experimental findings. In addition, we show how the developed framework enables the study of complicated transitions like the first step of a nonenzymatic DNA nucleoside synthesis in an aqueous environment, where the molecular fragmentation problem of earlier nanoreactor approaches is avoided.
