title: Electromagnetic study of the chlorosome antenna complex of Chlorobium tepidum.
abstract: Green sulfur bacteria are an iconic example of nature's adaptation: thriving in environments of extremely low photon density, the bacterium ranks itself among the most efficient natural light-harvesting organisms. The photosynthetic antenna complex of this bacterium is a self-assembled nanostructure, ≈60 × 150 nm, made of bacteriochlorophyll molecules. We study the system from a computational nanoscience perspective by using electrodynamic modeling with the goal of understanding its role as a nanoantenna. Three different nanostructures, built from two molecular packing moieties, are considered: a structure built of concentric cylinders of aggregated bacteriochlorophyll d monomers, a single cylinder of bacteriochlorophyll c monomers, and a model for the entire chlorosome. The theoretical model captures both coherent and incoherent components of exciton transfer. The model is employed to extract optical spectra, concentration and depolarization of electromagnetic fields within the chlorosome, and fluxes of energy transfer for the structures. The second model nanostructure shows the largest field enhancement. Further, field enhancement is found to be more sensitive to dynamic noise rather than structural disorder. Field depolarization, however, is similar for all structures. This indicates that the directionality of transfer is robust to structural variations, while on the other hand, the intensity of transfer can be tuned by structural variations.
authors.affiliation: Department of Chemistry and Chemical Biology, Harvard University , Cambridge, Massachusetts 02138, United States.
authors.forename: Stéphanie
authors.initials: S
authors.lastname: Valleau
authors.forename: Semion K
authors.initials: SK
authors.lastname: Saikin
authors.forename: Davood
authors.initials: D
authors.lastname: Ansari-Oghol-Beig
authors.forename: Masoud
authors.initials: M
authors.lastname: Rostami
authors.forename: Hossein
authors.initials: H
authors.lastname: Mossallaei
authors.forename: Alán
authors.initials: A
authors.lastname: Aspuru-Guzik
mesh_terms: D000465:Algorithms; D001426:Bacterial Proteins / Q000378:metabolism; D001429:Bacteriochlorophylls / Q000378:metabolism; D041883:Chlorobium / Q000201:enzymology*; D055590:Electromagnetic Phenomena; D004735:Energy Transfer; D045342:Light-Harvesting Protein Complexes / Q000737:chemistry* / Q000378:metabolism*
chemical_list: D001426:Bacterial Proteins; D001429:Bacteriochlorophylls; D045342:Light-Harvesting Protein Complexes; C002084:bacteriochlorophyll c