DNA-Directed Artificial Light-Harvesting Antenna

Designing and constructing multichromophoric, artificial light-harvesting antennas with controlled interchromophore distances, orientations, and defined donor–acceptor ratios to facilitate efficient unidirectional energy transfer is extremely challenging. Here, we demonstrate the assembly of a serie...

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Published inJournal of the American Chemical Society Vol. 133; no. 31; pp. 11985 - 11993
Main Authors Dutta, Palash K, Varghese, Reji, Nangreave, Jeanette, Lin, Su, Yan, Hao, Liu, Yan
Format Journal Article
LanguageEnglish
Published United States American Chemical Society 10.08.2011
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Abstract Designing and constructing multichromophoric, artificial light-harvesting antennas with controlled interchromophore distances, orientations, and defined donor–acceptor ratios to facilitate efficient unidirectional energy transfer is extremely challenging. Here, we demonstrate the assembly of a series of structurally well-defined artificial light-harvesting triads based on the principles of structural DNA nanotechnology. DNA nanotechnology offers addressable scaffolds for the organization of various functional molecules with nanometer scale spatial resolution. The triads are organized by a self-assembled seven-helix DNA bundle (7HB) into cyclic arrays of three distinct chromophores, reminiscent of natural photosynthetic systems. The scaffold accommodates a primary donor array (Py), secondary donor array (Cy3) and an acceptor (AF) with defined interchromophore distances. Steady-state fluorescence analyses of the triads revealed an efficient, stepwise funneling of the excitation energy from the primary donor array to the acceptor core through the intermediate donor. The efficiency of excitation energy transfer and the light-harvesting ability (antenna effect) of the triads was greatly affected by the relative ratio of the primary to the intermediate donors, as well as on the interchromophore distance. Time-resolved fluorescence analyses by time-correlated single-photon counting (TCSPC) and streak camera techniques further confirmed the cascading energy transfer processes on the picosecond time scale. Our results clearly show that DNA nanoscaffolds are promising templates for the design of artificial photonic antennas with structural characteristics that are ideal for the efficient harvesting and transport of energy.
AbstractList Designing and constructing multichromophoric, artificial light-harvesting antennas with controlled interchromophore distances, orientations, and defined donor-acceptor ratios to facilitate efficient unidirectional energy transfer is extremely challenging. Here, we demonstrate the assembly of a series of structurally well-defined artificial light-harvesting triads based on the principles of structural DNA nanotechnology. DNA nanotechnology offers addressable scaffolds for the organization of various functional molecules with nanometer scale spatial resolution. The triads are organized by a self-assembled seven-helix DNA bundle (7HB) into cyclic arrays of three distinct chromophores, reminiscent of natural photosynthetic systems. The scaffold accommodates a primary donor array (Py), secondary donor array (Cy3) and an acceptor (AF) with defined interchromophore distances. Steady-state fluorescence analyses of the triads revealed an efficient, stepwise funneling of the excitation energy from the primary donor array to the acceptor core through the intermediate donor. The efficiency of excitation energy transfer and the light-harvesting ability (antenna effect) of the triads was greatly affected by the relative ratio of the primary to the intermediate donors, as well as on the interchromophore distance. Time-resolved fluorescence analyses by time-correlated single-photon counting (TCSPC) and streak camera techniques further confirmed the cascading energy transfer processes on the picosecond time scale. Our results clearly show that DNA nanoscaffolds are promising templates for the design of artificial photonic antennas with structural characteristics that are ideal for the efficient harvesting and transport of energy.
Author Dutta, Palash K
Liu, Yan
Yan, Hao
Varghese, Reji
Nangreave, Jeanette
Lin, Su
AuthorAffiliation Arizona State University
AuthorAffiliation_xml – name: Arizona State University
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  givenname: Palash K
  surname: Dutta
  fullname: Dutta, Palash K
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  givenname: Reji
  surname: Varghese
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  givenname: Jeanette
  surname: Nangreave
  fullname: Nangreave, Jeanette
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  givenname: Su
  surname: Lin
  fullname: Lin, Su
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  givenname: Hao
  surname: Yan
  fullname: Yan, Hao
– sequence: 6
  givenname: Yan
  surname: Liu
  fullname: Liu, Yan
  email: yan_liu@asu.edu
BackLink https://www.ncbi.nlm.nih.gov/pubmed/21714548$$D View this record in MEDLINE/PubMed
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Snippet Designing and constructing multichromophoric, artificial light-harvesting antennas with controlled interchromophore distances, orientations, and defined...
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SubjectTerms DNA - chemistry
Energy Transfer
Fluorescent Dyes - chemistry
Light
Nanotechnology
Pyrenes - chemistry
Time Factors
Title DNA-Directed Artificial Light-Harvesting Antenna
URI http://dx.doi.org/10.1021/ja1115138
https://www.ncbi.nlm.nih.gov/pubmed/21714548
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