Quantum redirection of antenna absorption to photosynthetic reaction centres

Abstract

The early steps of photosynthesis involve the photo-excitation of reaction centres (RCs) and light-harvesting (LH) units. Here, we show that the --historically overlooked-- excitonic delocalisation across RC and LH pigments results in a redistribution of dipole strengths that benefits the absorption cross section of the optical bands associated with the RC of several species. While we prove that this redistribution is robust to the microscopic details of the dephasing between these units in the purple bacterium Rhodospirillum rubrum, we are able to show that the redistribution witnesses a more fragile, but persistent, coherent population dynamics which directs excitations from the LH towards the RC units under incoherent illumination and physiological conditions. Stochastic optimisation allows us to delineate clear guidelines and develop simple analytic expressions, in order to achieve directed coherent population dynamics in artificial nano-structures.

16 pages, Main text and Supplementary Information, 8 figures

References in corpus (5)

• Environment-Assisted Quantum Walks in Photosynthetic Energy Transfer
• Dephasing assisted transport: Quantum networks and biomolecules
• Efficiency of energy transfer in a light-harvesting system under quantum coherence
• The fundamental role of quantized vibrations in coherent light harvesting by cryptophyte algae
• Mapping The Ultrafast Flow Of Harvested Solar Energy In Living Photosynthetic Cells

Cited by in corpus (9)

• Cooperative quantum phenomena in light-matter platforms
• A cyanine dye rotaxane porphyrin nanoring complex as a model light harvesting system
• Using Fluorescence Detected Two-Dimensional Spectroscopy to Investigate Initial Exciton Delocalization Between Coupled Chromophores
• Design principles for long-range energy transfer at room temperature
• Efficient frequency-selective single-photon antennas based on a bio-inspired nano-scale atomic ring design with 9-fold symmetry
• Cavity-modified exciton dynamics in photosynthetic units
• Efficient long-distance energy transport in molecular systems through adiabatic passage
• Nonequilibrium steady-state picture of incoherent light-induced excitation harvesting
• Optical Properties of Concentric Nanorings of Quantum Emitters