walsh-facetselectivityin-2015.pdf (973.19 kB)
Facet selectivity in gold binding peptides: exploiting interfacial water structure
journal contribution
posted on 2015-01-01, 00:00 authored by L B Wright, Jesus Pablo Palafox-Hernandez, P M Rodger, S Corni, Tiffany WalshTiffany WalshPeptide sequences that can discriminate between gold facets under aqueous conditions offer a promising route to control the growth and organisation of biomimetically-synthesised gold nanoparticles. Knowledge of the interplay between sequence, conformations and interfacial properties is essential for predictable manipulation of these biointerfaces, but the structural connections between a given peptide sequence and its binding affinity remain unclear, impeding practical advances in the field. These structural insights, at atomic-scale resolution, are not easily accessed with experimental approaches, but can be delivered via molecular simulation. A current unmet challenge lies in forging links between predicted adsorption free energies derived from enhanced sampling simulations with the conformational ensemble of the peptide and the water structure at the surface. To meet this challenge, here we use an in situ combination of Replica Exchange with Solute Tempering with Metadynamics simulations to predict the adsorption free energy of a gold-binding peptide sequence, AuBP1, at the aqueous Au(111), Au(100)(1 × 1) and Au(100)(5 × 1) interfaces. We find adsorption to the Au(111) surface is stronger than to Au(100), irrespective of the reconstruction status of the latter. Our predicted free energies agree with experiment, and correlate with trends in interfacial water structuring. For gold, surface hydration is predicted as a chief determining factor in peptide-surface recognition. Our findings can be used to suggest how shaped seed-nanocrystals of Au, in partnership with AuBP1, could be used to control AuNP nanoparticle morphology.
History
Journal
Chemical scienceVolume
6Issue
9Pagination
5204 - 5214Publisher
Royal Society of ChemistryLocation
Cambridge, Eng.Publisher DOI
ISSN
2041-6520eISSN
2041-6539Language
engPublication classification
C Journal article; C1 Refereed article in a scholarly journalCopyright notice
2015, The AuthorsUsage metrics
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