The theory of dissipative exciton motion in chromophore complexes is applied to develop an approx... more The theory of dissipative exciton motion in chromophore complexes is applied to develop an approximate scheme for the simulation of frequency-domain linear absorption and circular dichroism. Besides lifetime broadening of the exciton lines and the inclusion of vibrational satellites in the spectra, the computations also account for static disorder. In applying the theory to a pigment protein complex of the photosynthetic light harvesting complex LHC-II of green plants the temperature dependence of linear absorption can be well reproduced. PACS numbers: 87.15.Aa In simulating the optical absorption of dye aggregates or chromophore complexes, one is confronted with the interplay of two distinct interactions: the coupling of electronic excitations to vibrational degrees of freedom and the interaction among the electronic excitations. Combining both couplings in a proper way should enable one to relate the absorption line shape to structural data.
A theory for calculating time-and frequency-domain optical spectra of pigment-protein complexes i... more A theory for calculating time-and frequency-domain optical spectra of pigment-protein complexes is presented using a density matrix approach. Non-Markovian effects in the excitonvibrational coupling are included. A correlation function is deduced from the simulation of 1.6 K fluorescence line narrowing spectra of a monomer pigment-protein complex ͑B777͒, and then used to calculate fluorescence line narrowing spectra of a dimer complex ͑B820͒. A vibrational sideband of an excitonic transition is obtained, a distinct non-Markovian feature, and agrees well with experiment on B820 complexes. The theory and the above correlation function are used elsewhere to make predictions and compare with data on time-domain pump-probe spectra and frequencydomain linear absorption, circular dichroism and fluorescence spectra of Photosystem II reaction centers.
A theory for electron transfer through a donor-bridge-acceptor system is described that involves ... more A theory for electron transfer through a donor-bridge-acceptor system is described that involves tunneling and hopping-like transfers and an intermediate regime. The theory considers how a delocalization of electronic states and static and dynamic disorder in electronic energies influence the charge transfer rate and is used to study experiments on hole transfer through DNA. While an exponential distance dependence of the yield of hole trapping is observed experimentally for small bridges, the yield for long bridges is reported to be almost distance-independent. For long bridge lengths, for which thermally activating hopping dominates over tunneling, the model considers two competing channels, a hopping via localized states and a transfer through partly delocalized states. The variable-range hopping mechanism and the delocalized states aspect of the theory are used to interpret the flat rather than a slow decrease of yield with increasing distance reported in experiments with long bridges. Renger and Marcus
The theory of dissipative exciton motion in chromophore complexes is applied to develop an approx... more The theory of dissipative exciton motion in chromophore complexes is applied to develop an approximate scheme for the simulation of frequency-domain linear absorption and circular dichroism. Besides lifetime broadening of the exciton lines and the inclusion of vibrational satellites in the spectra, the computations also account for static disorder. In applying the theory to a pigment protein complex of the photosynthetic light harvesting complex LHC-II of green plants the temperature dependence of linear absorption can be well reproduced. PACS numbers: 87.15.Aa In simulating the optical absorption of dye aggregates or chromophore complexes, one is confronted with the interplay of two distinct interactions: the coupling of electronic excitations to vibrational degrees of freedom and the interaction among the electronic excitations. Combining both couplings in a proper way should enable one to relate the absorption line shape to structural data.
A theory for calculating time-and frequency-domain optical spectra of pigment-protein complexes i... more A theory for calculating time-and frequency-domain optical spectra of pigment-protein complexes is presented using a density matrix approach. Non-Markovian effects in the excitonvibrational coupling are included. A correlation function is deduced from the simulation of 1.6 K fluorescence line narrowing spectra of a monomer pigment-protein complex ͑B777͒, and then used to calculate fluorescence line narrowing spectra of a dimer complex ͑B820͒. A vibrational sideband of an excitonic transition is obtained, a distinct non-Markovian feature, and agrees well with experiment on B820 complexes. The theory and the above correlation function are used elsewhere to make predictions and compare with data on time-domain pump-probe spectra and frequencydomain linear absorption, circular dichroism and fluorescence spectra of Photosystem II reaction centers.
A theory for electron transfer through a donor-bridge-acceptor system is described that involves ... more A theory for electron transfer through a donor-bridge-acceptor system is described that involves tunneling and hopping-like transfers and an intermediate regime. The theory considers how a delocalization of electronic states and static and dynamic disorder in electronic energies influence the charge transfer rate and is used to study experiments on hole transfer through DNA. While an exponential distance dependence of the yield of hole trapping is observed experimentally for small bridges, the yield for long bridges is reported to be almost distance-independent. For long bridge lengths, for which thermally activating hopping dominates over tunneling, the model considers two competing channels, a hopping via localized states and a transfer through partly delocalized states. The variable-range hopping mechanism and the delocalized states aspect of the theory are used to interpret the flat rather than a slow decrease of yield with increasing distance reported in experiments with long bridges. Renger and Marcus
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Papers by Thomas Renger