title: Fast delocalization leads to robust long-range excitonic transfer in a large quantum chlorosome model.
abstract: Chlorosomes are efficient light-harvesting antennas containing up to hundreds of thousands of bacteriochlorophyll molecules. With massively parallel computer hardware, we use a nonperturbative stochastic Schrödinger equation, while including an atomistically derived spectral density, to study excitonic energy transfer in a realistically sized chlorosome model. We find that fast short-range delocalization leads to robust long-range transfer due to the antennae's concentric-roll structure. Additionally, we discover anomalous behavior arising from different initial conditions, and outline general considerations for simulating excitonic systems on the nanometer to micrometer scale.
authors.affiliation: Department of Chemistry and Chemical Biology, Harvard University , 12 Oxford Street, Cambridge, Massachusetts 02138, United States.
authors.forename: Nicolas P D
authors.initials: NP
authors.lastname: Sawaya
authors.forename: Joonsuk
authors.initials: J
authors.lastname: Huh
authors.forename: Takatoshi
authors.initials: T
authors.lastname: Fujita
authors.forename: Semion K
authors.initials: SK
authors.lastname: Saikin
authors.forename: Alán
authors.initials: A
authors.lastname: Aspuru-Guzik
keywords: Chlorosome; exciton; graphics processing unit; green sulfur bacteria; photosynthesis; spectral density