Atomistic modelling of light-harvesting complexes:
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| Ulrich Kleinekathöfer | |
| Jacobs University Bremen | |
| The light absorption in light-harvesting complexes is performed by chlorophyll molecules. Recent experimental findings in some of these complexes suggest the existence of long-lived coherences between the individual pigments at low temperatures. In this context the question arises if the bath-induced fluctuations at different chromophores are spatially correlated or not. To this end we performed classicalmolecular dynamics simulations and quantum chemistry calculations on some light-harvesting systems. In these investigations at ambient temperatures, only weak correlations between the movements of the chromophores were detected at the atomic level. Furthermore two strategies will be outlined how to use the input from the atomistic simulations to study the transfer of energy in light-harvesting systems. On top of this, the same techniques can be employed to determine two-dimensional spectra which can be directly linked to experiment.
C. Olbrich, J. Strümpfer, K. Schulten, and U. Kleinekathöfer, Theory and Simulation of the Environmental Effects on FMO Electronic Transitions, J. Phys. Chem. Lett. 2, 1771–1776 (2011) C. Olbrich, Th. la Cour Jansen, J. Liebers, M. Aghtar, J. Strümpfer, K. Schulten, J. Knoester, and U. Kleinekathöfer, From Atomistic Modeling to Excitation Transfer and Two-Dimensional Spectra of the FMO Light-Harvesting Complex, J. Phys. Chem. B 115, 8609–8621(2011) C. Olbrich, J. Strümpfer, K. Schulten, and U. Kleinekathöfer, Quest for Spatially Correlated Fluctuations in the FMO Light-Harvesting Complex, J. Phys. Chem. B 115, 758-764 (2011) C. Olbrich and U. Kleinekathöfer, Time-dependent atomistic view on the electronic relaxation in light-harvesting system II, J. Phys. Chem. B 114, 12427–12437 (2010) |