Journal of Physical Chemistry, Vol.100, No.39, 15654-15662, 1996
Dissipative Exciton Motion in a Chlorophyll-A/B Dimer of the Light-Harvesting Complex of Photosystem-II - Simulation of Pump-Probe Spectra
The ultrafast dissipative exciton motion in a molecular dimer of the light harvesting complex II of higher plants is investigated theoretically. The density matrix formalism is applied to simulate the one- and two-color pump-probe spectra measured by Bittner ct al.(1) To incorporate coherent vibrational motion we use a representation in localized exciton vibrational states. The observed ultrafast transfer dynamics on the subpicosecond time scale can be well explained by means of a delocalization of the exciton wave function over both monomers. For the low-temperature one-color pump-probe measurement we predict quantum beats in the signal due to coherent nuclear wave packet motion. Furthermore, our calculations support the in-line geometry for the Chlorophyll a/b dimers in the pigment-protein complex.
Keywords:EXCITATION-ENERGY TRANSFER;LHC-II;FEMTOSECOND SPECTROSCOPY;RHODOBACTER-SPHAEROIDES;VIBRATIONAL DYNAMICS;ROOM-TEMPERATURE;PROTEIN COMPLEX;ANTENNA COMPLEX;MEMBRANE;TRIMERS