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Nat Mater. 2018 Feb;17(2):159-166. doi: 10.1038/nmat5033. Epub 2017 Nov 13.

Programmed coherent coupling in a synthetic DNA-based excitonic circuit.

Author information

1
Department of Biological Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
2
MIT-Harvard Center for Excitonics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
3
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, USA.
4
Center for Innovation in Medicine, The Biodesign Institute, Arizona State University, Tempe, Arizona 85287, USA.
5
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
6
School of Molecular Sciences, Arizona State University, Tempe, Arizona 85287, USA.
7
Center for Molecular Design and Biomimetics, The Biodesign Institute, Arizona State University, Tempe, Arizona 85287, USA.

Abstract

Natural light-harvesting systems spatially organize densely packed chromophore aggregates using rigid protein scaffolds to achieve highly efficient, directed energy transfer. Here, we report a synthetic strategy using rigid DNA scaffolds to similarly program the spatial organization of densely packed, discrete clusters of cyanine dye aggregates with tunable absorption spectra and strongly coupled exciton dynamics present in natural light-harvesting systems. We first characterize the range of dye-aggregate sizes that can be templated spatially by A-tracts of B-form DNA while retaining coherent energy transfer. We then use structure-based modelling and quantum dynamics to guide the rational design of higher-order synthetic circuits consisting of multiple discrete dye aggregates within a DX-tile. These programmed circuits exhibit excitonic transport properties with prominent circular dichroism, superradiance, and fast delocalized exciton transfer, consistent with our quantum dynamics predictions. This bottom-up strategy offers a versatile approach to the rational design of strongly coupled excitonic circuits using spatially organized dye aggregates for use in coherent nanoscale energy transport, artificial light-harvesting, and nanophotonics.

PMID:
29180771
DOI:
10.1038/nmat5033

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