Dresden 2009 – scientific programme
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BP: Fachverband Biologische Physik
BP 26: Photobiophysics
BP 26.6: Talk
Friday, March 27, 2009, 12:15–12:30, ZEU 260
Multidimensional Optical Probes of Electronic Correlations and Exciton Dynamics in Photosynthetic Complexes — •Dmitri V. Voronine1, Darius Abramavicius2, and Shaul Mukamel2 — 1Institut für Physikalische Chemie, Am Hubland, Universität Würzburg, Würzburg, Germany — 2Department of Chemistry, University of California, Irvine, USA
We simulate the multidimensional electronic chirality-induced (2D ECI) signals of excitons in the photosynthetic Fenna-Matthews-Olson (FMO) complexes from two species of green sulfur bacteria Chlorobium tepidum (C.t.) and Prosthecochloris aestuarii (P.a.). The spectra provide sensitive probes of local protein environment of the constituent bacteriochlorophyll a chromophores and reflect electronic structure variations (site energies and couplings) of the two complexes. Pulse polarization configurations are designed which can separate the coherent and incoherent exciton dynamics. Two main energy transfer pathways are revealed by varying the middle time delay in t2-dependent electronic 2D ECI spectra of FMO. Using coherent control we demonstrate optimal laser polarization configurations which enhance chirality-sensitive spectral features, revealing a slow energy transfer pathway which was not resolved in the non-chiral spectra. We show that coherent control can be used to optimize the resolution of cross-peaks and corresponding energy transfer pathways in 2D optical spectroscopy.