Quantum Pathways to Photosynthesis - Purpose-Driven Theoretical Chemistry for the Artificial Leaf

Grunddaten zu diesem Projekt

Beschreibung

Photosynthesis forms the basis for the majority of energy resources available on earth. But due to the complexity of photosystems and light-harvesting antenna involved, many details of energy-transfer and dissipation mechanisms, as well as subsequent reaction pathways in photosynthetic systems are still not well understood. Since these processes govern the overall efficiency of natural as well as of artificial solar energy conversion systems, their understanding is decisive for one of today's most ambitious research goals, namely the design of an artificial leaf. The aim of this research proposal is the development of autofocusing, property-oriented computer algorithms for the quantum chemical identification, analysis, and interpretation of the fundamental mechanisms in functional photosynthetic devices. This matches my long-term research goal, which is a bottom-up approach to biomimetic solar energy conversion based on systematic guidelines derived from first principles. The focus of this research programme will be on the design of purpose-driven quantum chemical methods for the investigation of photosystems in close connection to experimental data. This involves computer algorithms for the selective determination of electronic and vibronic interactions in photosynthetic reaction centers and light-harvesting systems from quantum chemical methods. These developments shall allow to determine spectroscopic signatures due to cooperative phenomena, from which important insight into electron- and energy-transfer pathways can be gained. By exploiting the subsystem structure of the entities under study, the development of theoretical methods for multi-dimensional optical spectroscopy of entire light-harvesting complexes shall be facilitated. Additionally, it is planned to extend the subsystem-based approaches to transient species occurring in photosynthetic systems after initial charge separation. Based on such methods a profound theoretical understanding of the molecular processes underlying photosynthesis shall be achieved, which opens up the way for a rational design of artificial photosynthetic systems.