Mode-selective chemistry and quantum state resolved polyatomic reaction dynamics

• Applicant: Professor Dr. Uwe Manthe
• Subject Area: Theoretical Chemistry: Electronic Structure, Dynamics, Simulation
• Term: from 2014 to 2021
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 261376728

The project studies the quantum state-specific dynamics of polyatomic reactions and intends to develop concepts to understand the mode-selective chemistry occurring in these systems. While a fully quantum state resolved level of understanding has been achieved for triatomic and selected tetratomic reactions, extending this level of understanding towards reactions involving a larger number of atoms is a challenging subject. Reactions of methane with atoms or diatomic molecules, e.g., H, Cl, O, or OH, are important processes in atmospheric and combustion chemistry. They are also prototypical polyatomic reactions extensively studied by fundamental research focusing on the detailed understanding of chemical reactivity. Impressive progress was achieved in experimental studies which demonstrated the mode-selective chemistry occurring in these systems. However, theoretical investigation are mostly based on reduced-dimensional models or quasi-classical trajectory simulations. In this project accurate full-dimensional quantum dynamics methods are used to study the reactions of methane with H, Cl, and OH. Specifically, wave packet dynamics calculations utilizing the multi-layer multi-configurational time-dependent Hartree approach and flux correlation functions will be employed to facilitate the detailed investigation of these six and seven atom reactions. The results will be compared to experimental observations. The central aim is the development of general concepts for the understanding of the mode-selective chemistry in polyatomic reactions.

• DFG Programme: Research Grants