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Programmed coherent coupling in a synthetic DNA-based excitonic circuit

Nature materials, 2018-02, Vol.17 (2), p.159-166 [Peer Reviewed Journal]

Copyright Nature Publishing Group Feb 2018 ;ISSN: 1476-1122 ;EISSN: 1476-4660 ;DOI: 10.1038/NMAT5033 ;PMID: 29180771

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Title:
Programmed coherent coupling in a synthetic DNA-based excitonic circuit
Author: Boulais, Étienne ; Sawaya, Nicolas P D ; Veneziano, Rémi ; Andreoni, Alessio ; Banal, James L ; Kondo, Toru ; Mandal, Sarthak ; Lin, Su ; Schlau-Cohen, Gabriela S ; Woodbury, Neal W ; Yan, Hao ; Aspuru-Guzik, Alán ; Bathe, Mark
Subjects: Absorption spectra ; Aggregates ; Chromophores ; Circuit design ; Coherence ; Cyanine dyes ; Deoxyribonucleic acid ; Dichroism ; DNA ; DNA - chemistry ; Energy consumption ; Energy harvesting ; Energy transfer ; Excitons ; Natural lighting ; Nucleic Acid Conformation ; Optics and Photonics - methods ; Quantum theory ; Scaffolds ; solar (photovoltaic), solid state lighting, photosynthesis (natural and artificial), charge transport, optics, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing) ; Transport properties
Is Part Of: Nature materials, 2018-02, Vol.17 (2), p.159-166
Description: 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.
Publisher: England: Nature Publishing Group
Language: English
Identifier: ISSN: 1476-1122
EISSN: 1476-4660
DOI: 10.1038/NMAT5033
PMID: 29180771
Source: MEDLINE
ProQuest Central

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Programmed coherent coupling in a synthetic DNA-based excitonic circuit

Copyright Nature Publishing Group Feb 2018 ;ISSN: 1476-1122 ;EISSN: 1476-4660 ;DOI: 10.1038/NMAT5033 ;PMID: 29180771

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