期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 9, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202116783
关键词
Chromophore assembly; Merocyanine; Nucleic acids; Nucleobase analogue; Supramolecular element
资金
- Bavarian State Ministry of Science and the Arts
- ERC [682586]
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [444286426]
- Projekt DEAL
- European Research Council (ERC) [682586] Funding Source: European Research Council (ERC)
This study reports the tuning of exciton coupling by changing the double helix conformation. Different arrangements of dyes were achieved by changing the backbone constitution and geometry of nucleic acids, resulting in distinct optical characteristics.
Exciton coupling between two or more chromophores in a specific environment is a key mechanism associated with color tuning and modulation of absorption energies. This concept is well exemplified by natural photosynthetic proteins, and can also be achieved in synthetic nucleic acid nanostructures. Here we report the coupling of barbituric acid merocyanine (BAM) nucleoside analogues and show that exciton coupling can be tuned by the double helix conformation. BAM is a nucleobase mimic that was incorporated in the phosphodiester backbone of RNA, DNA and GNA oligonucleotides. Duplexes with different backbone constitutions and geometries afforded different mutual dye arrangements, leading to distinct optical signatures due to competing modes of chromophore organization via electrostatic, dipolar, pi-pi-stacking and hydrogen-bonding interactions. The realized supramolecular motifs include hydrogen-bonded BAM-adenine base pairs and antiparallel as well as rotationally stacked BAM dieter aggregates with distinct absorption, CD and fluorescence properties.
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