Rocard, Lou, Wragg, Darren, Jobbins, Samuel A., Luciani, Lorenzo, Leoni, Stefano ![]() ![]() |
Preview |
PDF
- Accepted Post-Print Version
Download (3MB) | Preview |
Abstract
The use of a template bearing pre‐programmed receptor sites selectively accommodating chromophores at given positions is an attractive approach for engineering artificial light‐harvesting systems. Indulging this line of though, this work tackles the creation of tailored antenna architectures with yellow, red and blue chromophores exploiting three dynamic covalent reactions simultaneously, namely disulfide exchange, acyl hydrazone and boronic ester formations. The effect of various structural modifications, such as the chromophores as well as their spatial organization (distance, orientation, order), on the energy transfer within the antennas was studied by means of steady‐state UV‐Vis absorption and fluorescence spectroscopies. This systematic study allowed a significant improvement of the energy transfer efficiencies across the chromophores to a noticeable 22 and 15%, for the yellow and red donors to the blue acceptor, respectively. Metadynamics simulations suggested that the conformational properties of the antennas are driven by intramolecular chromophoric stacking interactions that, forcing the a‐helix to fold on itself, annul any effects deriving from the programming of the spatial arrangement of the receptor sides in the peptide backbone
Item Type: | Article |
---|---|
Date Type: | Published Online |
Status: | Published |
Schools: | Chemistry Advanced Research Computing @ Cardiff (ARCCA) |
Publisher: | Wiley |
ISSN: | 0947-6539 |
Date of First Compliant Deposit: | 5 September 2018 |
Date of Acceptance: | 20 August 2018 |
Last Modified: | 09 Jan 2024 18:07 |
URI: | https://orca.cardiff.ac.uk/id/eprint/114641 |
Citation Data
Cited 13 times in Scopus. View in Scopus. Powered By Scopus® Data
Actions (repository staff only)
![]() |
Edit Item |