Abstract
Abstract— Numerical simulations of the ultrafast exciton motion in photosynthetic antenna complexes are used to reproduce measured data of optical pump‐probe experiments. Emphasis is put on a chlorophyll aL/chlorophyll b dimer of the light‐harvesting complex of the photosystem II of higher plants (LHC‐II). To account for intramolecular excited‐state absorption the standard exciton theory is extended to the inclusion of a second higher excited singlet state per chlorophyll molecule. The density matrix theory is applied to describe the dissipative dynamics of excitons. Different mechanisms for energy relaxation and dephasing including pure dephasing processes are discussed. As a result, a further refinement of earlier calculations on the one‐color pump‐probe spectra at the LHC‐II can be presented. In particular, the presence of non‐Markovian effects with respect to the exciton‐vibrational interaction in the LHC‐II, discovered previously in the two‐color pump‐probe spectrum, is demonstrated here for the one‐color pump‐probe case.
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