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Templated chromophore assembly on peptide scaffolds: a structural evolution

Rocard, Lou, Wragg, Darren, Jobbins, Samuel A., Luciani, Lorenzo, Leoni, Stefano, Wouters, Johan and Bonifazi, Davide 2018. Templated chromophore assembly on peptide scaffolds: a structural evolution. Chemistry - A European Journal , -. 10.1002/chem.201803205

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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: 17 Oct 2019 19:03
URI: http://orca.cf.ac.uk/id/eprint/114641

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