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

研究成果: Article査読

73 被引用数 (Scopus)

抄録

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.

本文言語English
ページ(範囲)159-166
ページ数8
ジャーナルNature Materials
17
2
DOI
出版ステータスPublished - 2018 2月 1
外部発表はい

ASJC Scopus subject areas

  • 化学 (全般)
  • 材料科学(全般)
  • 凝縮系物理学
  • 材料力学
  • 機械工学

フィンガープリント

「Programmed coherent coupling in a synthetic DNA-based excitonic circuit」の研究トピックを掘り下げます。これらがまとまってユニークなフィンガープリントを構成します。

引用スタイル