Physics – Chemical Physics
Scientific paper
2001-06-14
Physics
Chemical Physics
Scientific paper
10.1016/S0301-0104(01)00520-1
Using the reduced density matrix formalism the time dependence of the exciton scattering in light-harvesting ring systems of purple bacteria is calculated. In contrast to the work of Kumble and Hochstrasser (J. Chem. Phys. 109 (1998) 855) static disorder (fluctuations of the site energies) as well as dynamic disorder (dissipation) is taken into account. For the description of dissipation we use Redfield theory in exciton eigenstates without secular approximation. This is shown to be equivalent to the Markovian limit of Capek's theory in local states. Circular aggregates with 18 pigments are studied to model the B850 ring of bacteriochlorophyls within LH2 complexes. It can be demonstrated that the dissipation is important for the time-dependent anisotropy of the fluorescence. Smaller values of static disorder are sufficient to produce the same decay rates in the anisotropy in comparison with the results by Kumble and Hochstrasser.
Barvik Ivan
Herman Pavel
Kleinekathoefer Ulrich
Schreiber Michael
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