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Publication Details
AFRICAN RESEARCH NEXUS
SHINING A SPOTLIGHT ON AFRICAN RESEARCH
biochemistry, genetics and molecular biology
Deoxyribonucleic Acid Encoded and Size-Defined π-Stacking of Perylene Diimides
Journal of the American Chemical Society, Volume 144, No. 1, Year 2022
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Description
Natural photosystems use protein scaffolds to control intermolecular interactions that enable exciton flow, charge generation, and long-range charge separation. In contrast, there is limited structural control in current organic electronic devices such as OLEDs and solar cells. We report here the DNA-encoded assembly of π-conjugated perylene diimides (PDIs) with deterministic control over the number of electronically coupled molecules. The PDIs are integrated within DNA chains using phosphoramidite coupling chemistry, allowing selection of the DNA sequence to either side, and specification of intermolecular DNA hybridization. In this way, we have developed a "toolbox"for construction of any stacking sequence of these semiconducting molecules. We have discovered that we need to use a full hierarchy of interactions: DNA guides the semiconductors into specified close proximity, hydrophobic-hydrophilic differentiation drives aggregation of the semiconductor moieties, and local geometry and electrostatic interactions define intermolecular positioning. As a result, the PDIs pack to give substantial intermolecular πwave function overlap, leading to an evolution of singlet excited states from localized excitons in the PDI monomer to excimers with wave functions delocalized over all five PDIs in the pentamer. This is accompanied by a change in the dominant triplet forming mechanism from localized spin-orbit charge transfer mediated intersystem crossing for the monomer toward a delocalized excimer process for the pentamer. Our modular DNA-based assembly reveals real opportunities for the rapid development of bespoke semiconductor architectures with molecule-by-molecule precision. © 2021 The Authors. Published by American Chemical Society.
Authors & Co-Authors
Gorman, Jeffrey
United Kingdom, Cambridge
University of Cambridge
Orsborne, Sarah R.E.
United Kingdom, Cambridge
University of Cambridge
Sridhar, Akshay
Sweden, Solna
Science for Life Laboratory
Budden, Peter J.
United Kingdom, Cambridge
University of Cambridge
Panjwani, Naitik A.
Germany, Berlin
Freie Universität Berlin
Ryan, Seán T.J.
United Kingdom, Cambridge
University of Cambridge
De Ornellas, Sara
United Kingdom, Oxford
University of Oxford
El-Sagheer, Afaf Helmy
United Kingdom, Oxford
University of Oxford
Brown, Tom
United Kingdom, Oxford
University of Oxford
Behrends, Jan
Germany, Berlin
Freie Universität Berlin
Keyser, Ulrich Felix
United Kingdom, Cambridge
University of Cambridge
Rao, Akshay
United Kingdom, Cambridge
University of Cambridge
Collepardo-Guevara, Rosana
United Kingdom, Cambridge
University of Cambridge
Friend, Richard H.
United Kingdom, Cambridge
University of Cambridge
Auras, Florian
United Kingdom, Cambridge
University of Cambridge
Statistics
Citations: 11
Authors: 15
Affiliations: 6
Identifiers
Doi:
10.1021/jacs.1c10241
ISSN:
00027863
Research Areas
Cancer
Genetics And Genomics