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Circularly polarised luminescence in an RNA-based homochiral, self-repairing, coordination polymer hydrogel

Lookup NU author(s): Dr Osama El-ZubirORCiD, Dr Pablo Rojas Martinez, Dr Gema Dura, Lamia Al-Mahamad, Dr Thomas PopeORCiD, Professor Thomas Penfold, Dr Fabio Cucinotta, Dr Liam McGarry, Dr Ben Horrocks, Professor Andrew HoultonORCiD

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This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).


Abstract

The aqueous equimolar reaction of Ag(I) ions with the thionucleoside enantiomer (-)6-thioguanosine, ((-)6tGH), yields a one-dimensional coordination polymer {Ag(-)tG}n, the self-assembly of which generates left-handed helical chains. The resulting helicity induces an enhanced chiro-optical response compared to the parent ligand. DFT calculations indicate that this enhancement is due to delocalisation of the excited state along the helical chains, with 7 units being required to converge the calculated CD spectra. At concentrations ≥ 15 mmol l-1 reactions form a sample-spanning hydrogel which shows self-repair capabilities with instantaneous recovery in which the dynamic reversibility of the coordination chains appears to play a role. The resulting gel exhibits circularly polarised luminescence (CPL) with a large dissymmetry factor of -0.07 ± 0.01 at 735 nm, a phenomenon not previously observed for this class of coordination polymer.


Publication metadata

Author(s): El-Zubir O, Martinez PR, Dura G, Al-Mahamad LLG, Pope T, Penfold TJ, Mackenzie LE, Pal R, Mosely J, Cucinotta F, McGarry LF, Horrocks BR, Houlton A

Publication type: Article

Publication status: Published

Journal: Journal of Materials Chemistry C

Year: 2022

Volume: 10

Issue: 18

Pages: 7329-7335

Print publication date: 14/05/2022

Online publication date: 20/04/2022

Acceptance date: 11/04/2022

Date deposited: 21/04/2022

ISSN (print): 2050-7526

ISSN (electronic): 2050-7534

Publisher: Royal Society of Chemistry

URL: https://doi.org/10.1039/D2TC00366J

DOI: 10.1039/D2TC00366J


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Funding

Funder referenceFunder name
BB/S017615/1
BB/T009268/1
EP/P015395/1EPSRC
EP/T022442/1
EP/S015310/1EPSRC
H2020-MSCA-ITN-2016-INDEED 722176
H2020- MSCA-ITN-859752
HEL4CHIROLED
SBPLY/19/180501/000191
URF\R\191002

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