title: Programming Light-Harvesting Efficiency Using DNA Origami.
abstract: The remarkable performance and quantum efficiency of biological light-harvesting complexes has prompted a multidisciplinary interest in engineering biologically inspired antenna systems as a possible route to novel solar cell technologies. Key to the effectiveness of biological "nanomachines" in light capture and energy transport is their highly ordered nanoscale architecture of photoactive molecules. Recently, DNA origami has emerged as a powerful tool for organizing multiple chromophores with base-pair accuracy and full geometric freedom. Here, we present a programmable antenna array on a DNA origami platform that enables the implementation of rationally designed antenna structures. We systematically analyze the light-harvesting efficiency with respect to number of donors and interdye distances of a ring-like antenna using ensemble and single-molecule fluorescence spectroscopy and detailed Förster modeling. This comprehensive study demonstrates exquisite and reliable structural control over multichromophoric geometries and points to DNA origami as highly versatile platform for testing design concepts in artificial light-harvesting networks.
authors.affiliation: Cavendish Laboratory, University of Cambridge , Cambridge CB3 0HE, United Kingdom.
authors.forename: Elisa A
authors.initials: EA
authors.lastname: Hemmig
authors.affiliation: Cavendish Laboratory, University of Cambridge , Cambridge CB3 0HE, United Kingdom.
authors.forename: Celestino
authors.initials: C
authors.lastname: Creatore
authors.affiliation: Institut für Physikalische und Theoretische Chemie, TU Braunschweig , 38106 Braunschweig, Germany.
authors.forename: Bettina
authors.initials: B
authors.lastname: Wünsch
authors.affiliation: Institut für Physikalische und Theoretische Chemie, TU Braunschweig , 38106 Braunschweig, Germany.
authors.forename: Lisa
authors.initials: L
authors.lastname: Hecker
authors.affiliation: Cavendish Laboratory, University of Cambridge , Cambridge CB3 0HE, United Kingdom.
authors.forename: Philip
authors.initials: P
authors.lastname: Mair
authors.affiliation: Cavendish Laboratory, University of Cambridge , Cambridge CB3 0HE, United Kingdom.
authors.forename: M Andy
authors.initials: MA
authors.lastname: Parker
authors.affiliation: Computational Science Laboratory, Microsoft Research , Cambridge CB1 2FB, United Kingdom.
authors.forename: Stephen
authors.initials: S
authors.lastname: Emmott
authors.affiliation: Institut für Physikalische und Theoretische Chemie, TU Braunschweig , 38106 Braunschweig, Germany.
authors.forename: Philip
authors.initials: P
authors.lastname: Tinnefeld
authors.affiliation: Cavendish Laboratory, University of Cambridge , Cambridge CB3 0HE, United Kingdom.
authors.forename: Ulrich F
authors.initials: UF
authors.lastname: Keyser
authors.affiliation: Cavendish Laboratory, University of Cambridge , Cambridge CB3 0HE, United Kingdom.
authors.forename: Alex W
authors.initials: AW
authors.lastname: Chin
mesh_terms: D002232:Carbocyanines / Q000737:chemistry*; D004247:DNA / Q000737:chemistry*; D008027:Light; D055668:Photochemical Processes; D013050:Spectrometry, Fluorescence
chemical_list: D002232:Carbocyanines; C089187:cyanine dye 3; C085321:cyanine dye 5; D004247:DNA
keywords: DNA nanotechnology; DNA origami; Förster resonance energy transfer; artificial light-harvesting; fluorescence spectroscopy