Efficient algorithms for the simulation of the non-adiabatic exciton transfer dynamics in light-harvesting systems

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The capture of sunlight by light-harvesting complexes is the first step of photosynthesis in biological systems. In order to understand the subtle relationship between structure and function in light-harvesting complexes of photosynthetic systems, experimental data have to be augmented by computer simulations, which allow to elucidate a more detailed picture of the structure-function relationship and the mechanistic aspects of the processes used by these complexes for an efficient energy conversion. In the last years, major theoretical advances open the pathway for approaches to compute exciton transfer processes in a much more direct way. This concerns the development of fast and sufficiently accurate semi-empirical methods to describe the ground and excited states properties, combined into multi-scale approaches to address huge systems including their complex dynamical effects. In this proposal, we want to combine well balanced semi-empirical quantum chemistry with force field methods and non-adiabatic propagation approaches for the electronic degrees of freedom, which will allow to follow the exciton dynamics directly. Based on this combination, experimental observables will be computed for comparison and justification. We want to address several different systems, the LH2, LH3, FMO and PC612 complexes. Theses systems have been well studied experimentally so far, therefore they are ideal to benchmark out new approach and show, how simulation can add insights, which so far could not be gained experimentally. The major goal is to develop an reliable but yet efficient methodology, which can be applied to other biological and new artificial light-harvesting complexes.