Pairing Accuracy and Efficiency in a Multi-Reference Excited State Method Applicable in Non-Adiabatic Molecular Dynamics Simulations

• Applicant: Dr. Daniel Graf
• Subject Area: Theoretical Chemistry: Electronic Structure, Dynamics, Simulation
• Term: since 2022
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 498448112

The interaction between matter and light as well as the resulting excited state mechanisms form the basis of not only many fundamental processes in nature including photosynthesis and human vision, but also technical applications like photovoltaic systems and light-mediated hydrogen production. A deep understanding of these mechanisms is hence essential to unravel many secrets of nature and, furthermore, to promote technological developments necessary to tackle the major environmental challenges society faces already today.To gain such a fundamental understanding, computer-based molecular dynamics simulations are of great importance, since they are able to describe processes on the atomistic level that are unreachable for the classical experiment. In order to simulate these processes reliably, in turn, quantum mechanical electronic structure methods are necessary that are both accurate and highly efficient. However, pairing accuracy and efficiency in a universally applicable method is one of the greatest problems in quantum chemistry and still remains an unsolved problem, since even the most modern methods have deficiencies in terms of either their accuracy or their efficiency The proposed project is dedicated to exactly this problem and serves the development of an accurate and efficient electronic structure method that can be used in computer-based simulations of light-induced processes. The basis for these developments is formed by a novel methodology that constitutes an excellent starting point with respect to the defined goal. The further proceeding can be divided into three major steps: The first step focuses on increasing the efficiency of the method, since high efficiency not only forms a basic prerequisite for ist application in computer-based molecular dynamics simulations, but also allows for detailed benchmarking of the method. Such benchmarking is essential to ensure the accuracy and reliability of the approach also for problems of high complexity and hence constitutes the second step of the project. Finally, the third step is devoted to the development of the necessary ingredients for the method to be used in computer-based molecular dynamics simulations and in this way opens up new possibilities for detailed and reliable investigations on light-matter interactions of any kind.

• DFG Programme: WBP Fellowship
• International Connection: United Kingdom
• Host: Dr. Alex Thom