@article{f8ae368c9d784210be58a21c4c1697e4,
title = "Programmed coherent coupling in a synthetic DNA-based excitonic circuit",
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.",
author = "Etienne Boulais and Sawaya, {Nicolas P.D.} and R{\'e}mi Veneziano and Alessio Andreoni and Banal, {James L.} and Toru Kondo and Sarthak Mandal and Su Lin and Schlau-Cohen, {Gabriela S.} and Woodbury, {Neal W.} and Hao Yan and Al{\'a}n Aspuru-Guzik and Mark Bathe",
note = "Funding Information: This work received support to M.B., G.S.S.C. and A.A.-G. from the MIT Center for Excitonics, an Energy Frontier Research Center funded by the US Department of Energy under award DE-SC0001088. M.B. additionally acknowledges funding from ONR DURIP N00014-16-1-2506 and ONR N00014-16-1-2181. A portion of the simulations was performed on Harvard University's Odyssey cluster, supported by the Research Computing Group of the FAS Division of Science. Some of the hardware used was provided by Harvard University's CUDA Center of Excellence (CCOE) Program, sponsored by NVIDIA. N.S. acknowledges funding from the Smith Family Graduate Science and Engineering Fellowship. The Biophysical Instrumentation Facility for the Study of Complex Macromolecular Systems (NSF-0070319) is gratefully acknowledged. E.B. acknowledges funding from the Natural Sciences and Engineering Research Council of Canada (NSERC) Publisher Copyright: {\textcopyright} 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.",
year = "2018",
month = feb,
day = "1",
doi = "10.1038/NMAT5033",
language = "English",
volume = "17",
pages = "159--166",
journal = "Nature Materials",
issn = "1476-1122",
publisher = "Nature Publishing Group",
number = "2",
}