The remarkable performance and quantum efficiency of biological light-harvesting complexes has prompted a multidisciplinary interest in engineering biologically inspired antenna systems as a possible route to novel solar cell technologies. Key to the effectiveness of biological "nanomachines" in light capture and energy transport is their highly ordered nanoscale architecture of photoactive molecules. Recently, DNA origami has emerged as a powerful tool for organizing multiple chromophores with base-pair accuracy and full geometric freedom. Here, we present a programmable antenna array on a DNA origami platform that enables the implementation of rationally designed antenna structures. We systematically analyze the light-harvesting efficiency with respect to number of donors and interdye distances of a ring-like antenna using ensemble and single-molecule fluorescence spectroscopy and detailed Förster modeling. This comprehensive study demonstrates exquisite and reliable structural control over multichromophoric geometries and points to DNA origami as highly versatile platform for testing design concepts in artificial light-harvesting networks.A. W. C. acknowledges support from the Winton Programme for the Physics of Sustainability.
U. F. K. was partly supported by an ERC starting grant (PassMembrane, EY 261101).
E. A.H. acknowledges support from Janggen-Pöhn Stiftung and the Schweizerischer Nationalfonds
(SNF). P. T. acknowledges support by a starting grant (SiMBA, EU 261162) of the
European Research Council (ERC). B. W. gratefully acknowledges support by the Braunschweig
International Graduate School of Metrology B-IGSM and the DFG Research Training
Group GrK1952/1 ‘Metrology for Complex Nanosystems’. P. M. thankfully acknowledges the
support of the EPSRC Centre for Doctoral Training in Sensor Technologies and Applications
EP/L015889/1.This is the final version of the article. It first appeared from ACS via https://doi.org/10.1021/acs.nanolett.5b0513
