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Exciton Chirality Inversion in Dye Dimers Templated by DNA Holliday Junction

[Image: see text] While only one enantiomer of chiral biomolecules performs a biological function, access to both enantiomers (or enantiomorphs) proved to be advantageous for technology. Using dye covalent attachment to a DNA Holliday junction (HJ), we created two pairs of dimers of bis(chloroindole...

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Autores principales: Mass, Olga A., Basu, Shibani, Patten, Lance K., Terpetschnig, Ewald A., Krivoshey, Alexander I., Tatarets, Anatoliy L., Pensack, Ryan D., Yurke, Bernard, Knowlton, William B., Lee, Jeunghoon
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9706552/
https://www.ncbi.nlm.nih.gov/pubmed/36355575
http://dx.doi.org/10.1021/acs.jpclett.2c02721
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author Mass, Olga A.
Basu, Shibani
Patten, Lance K.
Terpetschnig, Ewald A.
Krivoshey, Alexander I.
Tatarets, Anatoliy L.
Pensack, Ryan D.
Yurke, Bernard
Knowlton, William B.
Lee, Jeunghoon
author_facet Mass, Olga A.
Basu, Shibani
Patten, Lance K.
Terpetschnig, Ewald A.
Krivoshey, Alexander I.
Tatarets, Anatoliy L.
Pensack, Ryan D.
Yurke, Bernard
Knowlton, William B.
Lee, Jeunghoon
author_sort Mass, Olga A.
collection PubMed
description [Image: see text] While only one enantiomer of chiral biomolecules performs a biological function, access to both enantiomers (or enantiomorphs) proved to be advantageous for technology. Using dye covalent attachment to a DNA Holliday junction (HJ), we created two pairs of dimers of bis(chloroindolenine)squaraine dye that enabled strongly coupled molecular excitons of opposite chirality in solution. The exciton chirality inversion was achieved by interchanging single covalent linkers of unequal length tethering the dyes of each dimer to the HJ core. Dimers in each pair exhibited profound exciton-coupled circular dichroism (CD) couplets of opposite signs. Dimer geometries, modeled by simultaneous fitting absorption and CD spectra, were related in each pair as nonsuperimposable and nearly exact mirror images. The origin of observed exciton chirality inversion was explained in the view of isomerization of the stacked Holliday junction. This study will open new opportunities for creating excitonic DNA-based materials that rely on programmable system chirality.
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spelling pubmed-97065522022-11-30 Exciton Chirality Inversion in Dye Dimers Templated by DNA Holliday Junction Mass, Olga A. Basu, Shibani Patten, Lance K. Terpetschnig, Ewald A. Krivoshey, Alexander I. Tatarets, Anatoliy L. Pensack, Ryan D. Yurke, Bernard Knowlton, William B. Lee, Jeunghoon J Phys Chem Lett [Image: see text] While only one enantiomer of chiral biomolecules performs a biological function, access to both enantiomers (or enantiomorphs) proved to be advantageous for technology. Using dye covalent attachment to a DNA Holliday junction (HJ), we created two pairs of dimers of bis(chloroindolenine)squaraine dye that enabled strongly coupled molecular excitons of opposite chirality in solution. The exciton chirality inversion was achieved by interchanging single covalent linkers of unequal length tethering the dyes of each dimer to the HJ core. Dimers in each pair exhibited profound exciton-coupled circular dichroism (CD) couplets of opposite signs. Dimer geometries, modeled by simultaneous fitting absorption and CD spectra, were related in each pair as nonsuperimposable and nearly exact mirror images. The origin of observed exciton chirality inversion was explained in the view of isomerization of the stacked Holliday junction. This study will open new opportunities for creating excitonic DNA-based materials that rely on programmable system chirality. American Chemical Society 2022-11-10 2022-11-24 /pmc/articles/PMC9706552/ /pubmed/36355575 http://dx.doi.org/10.1021/acs.jpclett.2c02721 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Mass, Olga A.
Basu, Shibani
Patten, Lance K.
Terpetschnig, Ewald A.
Krivoshey, Alexander I.
Tatarets, Anatoliy L.
Pensack, Ryan D.
Yurke, Bernard
Knowlton, William B.
Lee, Jeunghoon
Exciton Chirality Inversion in Dye Dimers Templated by DNA Holliday Junction
title Exciton Chirality Inversion in Dye Dimers Templated by DNA Holliday Junction
title_full Exciton Chirality Inversion in Dye Dimers Templated by DNA Holliday Junction
title_fullStr Exciton Chirality Inversion in Dye Dimers Templated by DNA Holliday Junction
title_full_unstemmed Exciton Chirality Inversion in Dye Dimers Templated by DNA Holliday Junction
title_short Exciton Chirality Inversion in Dye Dimers Templated by DNA Holliday Junction
title_sort exciton chirality inversion in dye dimers templated by dna holliday junction
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9706552/
https://www.ncbi.nlm.nih.gov/pubmed/36355575
http://dx.doi.org/10.1021/acs.jpclett.2c02721
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