Quantum dynamics studies of system-bath effects in charge- and energy-transfer processes

• Applicant: Professor Dr. Volker Engel
• Subject Area: Theoretical Chemistry: Electronic Structure, Dynamics, Simulation
• Term: from 2012 to 2019
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 207601309

In systematically varying the influence of a surrounding on (1) transfer processes and (2) on linear/non-linear spectra we aim at a deeper understanding of complex intra- and intermolecular dynamics in excited states of molecular aggregates.One important point is the dimer-based description of exciton-trapping processes which are of primary importance for the efficiency of organic photovoltaic devices and opto-electronics. This approach which was developed in the first funding period will be applied to other systems to investigate how general the identified mechanisms are. An essential goal is to develop a detailed picture of the competing intra-dimer relaxation dynamics and the inter-dimer energy transfer.The trapping processes within a dimer unit are connected to the localization of excitation energy on sub-units of aggregates and also to non-adiabatic transitions between excited states. Aspects like the dissipation-driven charge and energy transfer or the annihilation of excitons are to be characterized with the help of the underlying quantum dynamics.Another goal of is to advance the calculations of two-dimensional vibronic spectra. This includes the incorporation of various vibrational degrees of freedom and also the extension of the aggregate size. A central aspect is the coupling of coherent electronic and nuclear motion and the influence of a bath on this dynamics.

• DFG Programme: Research Units
• Subproject of: FOR 1809: Light-induced Dynamics in Molecular Aggregates