Programmed coherent coupling in a synthetic DNA-based excitonic circuit

Etienne Boulais, Nicolas P.D. Sawaya, Rémi Veneziano, Alessio Andreoni, James L. Banal, Toru Kondo, Sarthak Mandal, Su Lin, Gabriela S. Schlau-Cohen, Neal W. Woodbury, Hao Yan, Alán Aspuru-Guzik, Mark Bathe

Research output: Contribution to journalArticle

40 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)159-166
Number of pages8
JournalNature Materials
Volume17
Issue number2
DOIs
Publication statusPublished - Feb 1 2018

ASJC Scopus subject areas

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering

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    Boulais, E., Sawaya, N. P. D., Veneziano, R., Andreoni, A., Banal, J. L., Kondo, T., Mandal, S., Lin, S., Schlau-Cohen, G. S., Woodbury, N. W., Yan, H., Aspuru-Guzik, A., & Bathe, M. (2018). Programmed coherent coupling in a synthetic DNA-based excitonic circuit. Nature Materials, 17(2), 159-166. https://doi.org/10.1038/NMAT5033