Development and application of an ab initio Photo-Nanoreactor

从头算光纳米反应器的开发与应用

• 批准号: 419817859
• 负责人: Professor Dr. Jan Meisner
• 金额: --
• 依托单位: Department of Chemistry
• 依托单位国家: 德国
• 项目类别: Research Fellowships
• 财政年份: 2019
• 资助国家: 德国
• 起止时间: 2018-12-31 至 2021-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/419817859?language=en
• 关键词: Development; application; ab; initio; Photo

The automatized investigation of chemical reactions enables the creation of complex reaction networks and to identify unknown synthesis routes. The decisive advantage is that the exploration of chemcial reactivity is carried out without a priori assumptions and, thus, is independent of the expertise of the user. In this project, the ab initio nanoreactor, a concept of automatized reaction discovery deverloped in the group of Todd Martínez, will be extended to electronically excited states.The in this project newly developed ab initio photo-nanoreactor will enable the systematic investigation of photochemical reactivity of molecular systems. For that, state-of-the-art GPU accelerated electronic structure methods, such as CASSCF and FOMO-CASCI will be applied. For the description of the non-adiabatic molecular dynamics, ab initio-Mutiple-Spawning (AIMS) will be utilized. The capabilities of the ab initio photo-nanoreactor will be tested with familiar photochemical reactions like [2+2] photo-cycloadditions and photoisomerizations of unsaturated compounds. The photochemical synthesis of highly strained ring systems such as cubane derivates and ladderanes are possible applications.

化学反应的自动化研究能够创建复杂的反应网络并识别未知的合成路线。决定性的优点是，化学反应性的探索是在没有先验假设的情况下进行的，因此，是独立于用户的专业知识。在本计画中，由托德.马丁内兹（Martínez）等人所提出的自动化反应发现的概念--从头算奈米反应器（ab initio nanoreactor），将被延伸至电子激发态。本计画中新开发的从头算光奈米反应器（ab initio photo-nanoreactor），将能系统地研究分子系统的光化学反应性。为此，将应用最先进的GPU加速电子结构方法，如CASSCF和FOMO-CASCI。对于非绝热分子动力学的描述，将利用从头算多繁殖（AIMS）。从头算光纳米反应器的能力将与熟悉的光化学反应，如[2+2]光环加成和不饱和化合物的光异构化进行测试。高张力环体系如立方烷衍生物和梯形烷的光化学合成是可能的应用。

项目成果

Flyby reaction trajectories: Chemical dynamics under extrinsic force

• DOI: 10.1126/science.abi7609
• 发表时间: 2021-07-09
• 期刊: SCIENCE
• 影响因子: 56.9
• 作者: Liu, Yun;Holm, Soren;Moore, Jeffrey S.
• 通讯作者: Moore, Jeffrey S.