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Coupling to Charge Transfer States Is the Key to Modulate the Optical Bands for Efficient Light-Harvesting in Purple Bacteria.
摘要： The photosynthetic apparatus of purple bacteria uses exciton delocalization and static disorder to modulate the position and broadening of its absorption bands, leading to efficient light harvesting. Its main antenna complex, LH2, contains two rings of identical bacteriochlorophyll pigments, B800 and B850, absorbing at 800 nm and at 850 nm, respectively. It has been an unsolved problem why static disorder of the strongly coupled B850 ring is several times larger than that of the B800 ring. Here we show that mixing between excitons and charge transfer states in the B850 ring is responsible for the effect. The linear absorption spectrum of the LH2 system is simulated by using a multi-scale approach with an exciton Hamiltonian generalized to include the charge transfer states that involve adjacent pigment pairs, with static disorder modelled microscopically by molecular dynamics simulations. Our results show that a sufficient inhomogeneous broadening of the B850 band, needed for efficient light-harvesting, is only obtained by utilizing static disorder in the coupling between local excited and inter-pigment charge transfer states.
关键词： exciton delocalization,B850,B800,charge transfer states,purple bacteria,LH2,molecular dynamics simulations,static disorder,bacteriochlorophyll pigments,photosynthetic apparatus,light harvesting
更新于2025-09-10 09:29:36
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Probing Exciton Delocalization in Organic Semiconductors: Insight from Time-Resolved Electron Paramagnetic Resonance and Magnetophotoselection Experiments
摘要： Delocalization of excited states of organic semiconductors is directly related to their e?ciency in devices. Time-resolved electron paramagnetic resonance spectroscopy provides unique capabilities in this respect because of its high spectral resolution and capability to probe the geometry and extent of excitons. Using magnetophotoselection experiments, the mode of exciton delocalization, along the backbone or parallel to the π?π stacking direction of the conjugated polymers, can be revealed. We demonstrate the robustness of this approach by applying it to building blocks of a prototypical conjugated polymer showing a symmetry of their excited states being far from ideal for this experiment. This renders magnetophotoselection superior to other approaches because it is applicable to a wealth of other organic semiconductors. The insight gained into exciton delocalization is crucial to the structure?function relationship of organic semiconductors and directly relevant for developing highly e?cient materials.
关键词： time-resolved electron paramagnetic resonance,conjugated polymers,exciton delocalization,organic semiconductors,magnetophotoselection
更新于2025-09-09 09:28:46