Project coordinator: Oliver Kühn
Co-workers: Xiaomeng Liu, Per-Arno Plötz, Marco Schröter, Jan Schulze
Collaborations: Stefan Lochbrunner (Rostock), Jörg Megow (Potsdam), T. Pullerits (Lund), Thomas Niehaus (Lyon), Mohamed Shibl (Doha), Mohamed Al-Marri (Doha)

Project description

The exciton dynamics in light-harvesting complexes, that is the energy transfer from the absorption site(s) to the photosynthetic reaction center, is one of the most efficient processes in nature. It is of large interest to understand the mechanisms of this dynamics in order to improve artificial devices like organic solar cells. We apply wave-function (ML-MCTDH) and density matrix (Redfield, HEOM) based approaches to study both, the coherent and dissipative exciton transfer in photosynthetic light-harvesting as well as in man-made molecular aggregates. In particular we are interested in the influence of intra-molecular and environmental fluctuations (vibrations) on the dynamics, the spectroscopic features arising from different kinds of dynamics, and the interplay between structure and energy transfer mechanisms. For efficient determination of excitation energies, Coulomb couplings as well as their fluctuations, a self-consistent charge density functional tight-binding (SCC-DFTB) protocol is developed.

Publications

1. M. Schröter, S. D. Ivanov, J. Schulze, S. P. Polyutov, Y. Yan, T. Pullerits, O. Kühn
   Exciton-Vibrational Coupling in the Dynamics and Spectroscopy of Frenkel Excitons in Molecular Aggregates
   Physics Reports 567, 1 (2015)
   

2. J. Schulze, M. Shibl, M. Al-Marri, O. Kühn
   Multi-Layer Multi-Configuration Time-Dependent Hartree (ML-MCTDH) Approach to the Correlated Exciton-Vibrational Dynamics in the FMO Complex
   Journal of Chemical Physics 144, 185101 (2016)
   

3. P.-A. Plötz, T. Niehaus, O. Kühn
   A New Efficient Method for Calculation of Frenkel Exciton Parameters in Molecular Aggregates
   Journal of Chemical Physics 140, 174101 (2014)