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Programming Light-Harvesting Efficiency Using DNA Origami.

Published version
Peer-reviewed

Repository DOI


Change log

Authors

Hemmig, Elisa A 
Creatore, Celestino 
Wünsch, Bettina 
Hecker, Lisa 
Mair, Philip 

Abstract

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.

Description

Keywords

DNA nanotechnology, DNA origami, Förster resonance energy transfer, artificial light-harvesting, fluorescence spectroscopy, Carbocyanines, DNA, Light, Photochemical Processes, Spectrometry, Fluorescence

Journal Title

Nano Lett

Conference Name

Journal ISSN

1530-6984
1530-6992

Volume Title

16

Publisher

American Chemical Society (ACS)
Sponsorship
Engineering and Physical Sciences Research Council (EP/L015889/1)
European Research Council (261101)
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.