title: Robust excitons inhabit soft supramolecular nanotubes.
abstract: Nature's highly efficient light-harvesting antennae, such as those found in green sulfur bacteria, consist of supramolecular building blocks that self-assemble into a hierarchy of close-packed structures. In an effort to mimic the fundamental processes that govern nature's efficient systems, it is important to elucidate the role of each level of hierarchy: from molecule, to supramolecular building block, to close-packed building blocks. Here, we study the impact of hierarchical structure. We present a model system that mirrors nature's complexity: cylinders self-assembled from cyanine-dye molecules. Our work reveals that even though close-packing may alter the cylinders' soft mesoscopic structure, robust delocalized excitons are retained: Internal order and strong excitation-transfer interactions--prerequisites for efficient energy transport--are both maintained. Our results suggest that the cylindrical geometry strongly favors robust excitons; it presents a rational design that is potentially key to nature's high efficiency, allowing construction of efficient light-harvesting devices even from soft, supramolecular materials.
authors.affiliation: Center for Excitonics and Department of Chemistry and Eisele@ccny.cuny.edu Nicastro@brandeis.edu J.Knoester@rug.nl MGB@mit.edu.
authors.forename: Dörthe M
authors.initials: DM
authors.lastname: Eisele
authors.affiliation: Center for Excitonics and Department of Chemistry and Eisele@ccny.cuny.edu Nicastro@brandeis.edu J.Knoester@rug.nl MGB@mit.edu.
authors.forename: Dylan H
authors.initials: DH
authors.lastname: Arias
authors.affiliation: Biology Department, Rosenstiel Basic Medical Science Research Center, Brandeis University, Waltham, MA 02454;
authors.forename: Xiaofeng
authors.initials: X
authors.lastname: Fu
authors.affiliation: Institute for Theoretical Physics and Zernike Institute for Advanced Materials, University of Groningen, NL-9747 AG, Groningen, The Netherlands;
authors.forename: Erik A
authors.initials: EA
authors.lastname: Bloemsma
authors.affiliation: Center for Excitonics and Department of Chemistry and.
authors.forename: Colby P
authors.initials: CP
authors.lastname: Steiner
authors.affiliation: Center for Excitonics and Department of Chemistry and.
authors.forename: Russell A
authors.initials: RA
authors.lastname: Jensen
authors.affiliation: Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139;
authors.forename: Patrick
authors.initials: P
authors.lastname: Rebentrost
authors.affiliation: Institut für Festkörperphysik, Technische Universität Berlin, 103623 Berlin, Germany; and.
authors.forename: Holger
authors.initials: H
authors.lastname: Eisele
authors.affiliation: Department of Chemistry, University of Chicago, Chicago, IL 60637.
authors.forename: Andrei
authors.initials: A
authors.lastname: Tokmakoff
authors.affiliation: Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139;
authors.forename: Seth
authors.initials: S
authors.lastname: Lloyd
authors.affiliation: Center for Excitonics and Department of Chemistry and.
authors.forename: Keith A
authors.initials: KA
authors.lastname: Nelson
authors.affiliation: Biology Department, Rosenstiel Basic Medical Science Research Center, Brandeis University, Waltham, MA 02454; Eisele@ccny.cuny.edu Nicastro@brandeis.edu J.Knoester@rug.nl MGB@mit.edu.
authors.forename: Daniela
authors.initials: D
authors.lastname: Nicastro
authors.affiliation: Institute for Theoretical Physics and Zernike Institute for Advanced Materials, University of Groningen, NL-9747 AG, Groningen, The Netherlands; Eisele@ccny.cuny.edu Nicastro@brandeis.edu J.Knoester@rug.nl MGB@mit.edu.
authors.forename: Jasper
authors.initials: J
authors.lastname: Knoester
authors.affiliation: Center for Excitonics and Department of Chemistry and Eisele@ccny.cuny.edu Nicastro@brandeis.edu J.Knoester@rug.nl MGB@mit.edu.
authors.forename: Moungi G
authors.initials: MG
authors.lastname: Bawendi
mesh_terms: D002232:Carbocyanines / Q000737:chemistry; D004396:Coloring Agents / Q000737:chemistry; D008962:Models, Theoretical; D043942:Nanotubes
chemical_list: D002232:Carbocyanines; D004396:Coloring Agents
keywords: exciton theory; light-harvesting antennae systems; photosynthesis; self-assembled excitonic nanoscale systems; supramolecular assembly
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