title: Assembling programmable FRET-based photonic networks using designer DNA scaffolds.
abstract: DNA demonstrates a remarkable capacity for creating designer nanostructures and devices. A growing number of these structures utilize Förster resonance energy transfer (FRET) as part of the device's functionality, readout or characterization, and, as device sophistication increases so do the concomitant FRET requirements. Here we create multi-dye FRET cascades and assess how well DNA can marshal organic dyes into nanoantennae that focus excitonic energy. We evaluate 36 increasingly complex designs including linear, bifurcated, Holliday junction, 8-arm star and dendrimers involving up to five different dyes engaging in four-consecutive FRET steps, while systematically varying fluorophore spacing by Förster distance (R0). Decreasing R0 while augmenting cross-sectional collection area with multiple donors significantly increases terminal exciton delivery efficiency within dendrimers compared with the first linear constructs. Förster modelling confirms that best results are obtained when there are multiple interacting FRET pathways rather than independent channels by which excitons travel from initial donor(s) to final acceptor.
authors.affiliation: 1] Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, 4555 Overlook Avenue, South West, Washington DC, Washington 20375, USA [2] College of Science, George Mason University, 4400 University Drive, Fairfax, Virginia 22030, USA.
authors.forename: Susan
authors.initials: S
authors.lastname: Buckhout-White
authors.affiliation: Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, 4555 Overlook Avenue, South West, Washington DC, Washington 20375, USA.
authors.forename: Christopher M
authors.initials: CM
authors.lastname: Spillmann
authors.affiliation: 1] Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, 4555 Overlook Avenue, South West, Washington DC, Washington 20375, USA [2] Department of Chemistry, University of British Columbia, 2036 Main Mall, Vancouver, British Columbia V6T 1Z1, Canada.
authors.forename: W Russ
authors.initials: WR
authors.lastname: Algar
authors.affiliation: 1] Electronic Science and Technology Division, Code 6800, U.S. Naval Research Laboratory, 4555 Overlook Avenue, South West, Washington DC, Washington 20375, USA [2] Sotera Defense Solutions, Inc., 7230 Lee DeForest Drive, Columbia, Maryland 21046, USA.
authors.forename: Ani
authors.initials: A
authors.lastname: Khachatrian
authors.affiliation: Electronic Science and Technology Division, Code 6800, U.S. Naval Research Laboratory, 4555 Overlook Avenue, South West, Washington DC, Washington 20375, USA.
authors.forename: Joseph S
authors.initials: JS
authors.lastname: Melinger
authors.affiliation: Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, 4555 Overlook Avenue, South West, Washington DC, Washington 20375, USA.
authors.forename: Ellen R
authors.initials: ER
authors.lastname: Goldman
authors.affiliation: Electronic Science and Technology Division, Code 6800, U.S. Naval Research Laboratory, 4555 Overlook Avenue, South West, Washington DC, Washington 20375, USA.
authors.forename: Mario G
authors.initials: MG
authors.lastname: Ancona
authors.affiliation: Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, 4555 Overlook Avenue, South West, Washington DC, Washington 20375, USA.
authors.forename: Igor L
authors.initials: IL
authors.lastname: Medintz
mesh_terms: D002232:Carbocyanines / Q000032:analysis / Q000737:chemistry*; D004247:DNA / Q000737:chemistry*; D031541:Fluorescence Resonance Energy Transfer; D005456:Fluorescent Dyes / Q000032:analysis / Q000737:chemistry*; D007700:Kinetics; D016571:Neural Networks, Computer; D009690:Nucleic Acid Conformation; D017785:Photons; D013816:Thermodynamics
chemical_list: D002232:Carbocyanines; D005456:Fluorescent Dyes; D004247:DNA