Atomistic study of energy funneling in the light-harvesting complex of green sulfur bacteria
arXiv:1307.0886 · doi:10.1021/ja412035q
Abstract
Phototrophic organisms such as plants, photosynthetic bacteria and algae use microscopic complexes of pigment molecules to absorb sunlight. Within the light-harvesting complexes, which frequently have several functional and structural subunits, the energy is transferred in the form of molecular excitations with very high efficiency. Green sulfur bacteria are considered to be amongst the most efficient light-harvesting organisms. Despite multiple experimental and theoretical studies of these bacteria the physical origin of the efficient and robust energy transfer in their light-harvesting complexes is not well understood. To study excitation dynamics at the systems level we introduce an atomistic model that mimics a complete light-harvesting apparatus of green sulfur bacteria. The model contains approximately 4000 pigment molecules and comprises a double wall roll for the chlorosome, a baseplate and six Fenna-Matthews-Olson trimer complexes. We show that the fast relaxation within functional subunits combined with the transfer between collective excited states of pigments can result in robust energy funneling. Energy transfer is robust on the initial excitation conditions and temperature changes. Moreover, the same mechanism describes the coexistence of multiple timescales of excitation dynamics frequently observed in ultrafast optical experiments. While our findings support the hypothesis of supertransfer, the model reveals energy transport through multiple channels on different length scales.
15 pages, 14 figures
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- Linear-algebraic bath transformation for simulating complex open quantum systems
- Two-dimensional electronic spectra of the photosynthetic apparatus of green sulfur bacteria
- Macroscopic coherence as an emergent property in molecular nanotubes
- Superradiance at the localization-delocalization crossover in tubular chlorosomes
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- Bio-inspired natural sunlight-pumped lasers
- Diagrammatic quantum Monte Carlo toward the calculation of transport properties in disordered semiconductors
- Optical Spectra of p-Doped PEDOT Nano-Aggregates Provide Insight into the Material Disorder
- A stochastic reorganizational bath model for electronic energy transfer