Development and application of an ab initio Photo-Nanoreactor

化学反应的自动化研究使创建复杂的反应网络和识别未知的合成路线成为可能。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，因此不依赖于用户的专门知识。在这个项目中，从头算纳米反应器，一个自动化反应发现的概念，由Todd Martínez小组开发，将扩展到电子激发态。本项目新开发的从头算光纳米反应器将使分子体系光化学反应性的系统研究成为可能。为此，将采用最先进的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，将采用从头-多次繁殖（AIMS）方法。从头算光纳米反应器的性能将通过熟悉的光化学反应进行测试，如[2+2]光环加成和光异构化的不饱和化合物。高应变环系如立方烷衍生物和阶梯烷的光化学合成是可能的应用。

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.