Kinetically controlled coassembly of multichromophoric peptide hydrogelators and the impacts on energy transport

Herdeline Ardona, Emily Draper, Matthew Wallace, Francesca Citossi, Louise Serpell, Dave J. Adams, John D. Tovar

Research output: Contribution to journalArticlepeer-review

69 Citations (Scopus)
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Abstract

We report a peptide-based multichromophoric hydrogelator system, wherein π-electron units with different inherent spectral energies are spatially controlled within peptidic 1-D nanostructures to create localized energy gradients in aqueous environments. This is accomplished by mixing different π-conjugated peptides prior to initiating self-assembly through solution acidification. We can vary the kinetics of the assembly and the degree of self-sorting through the choice of the assembly trigger, which changes the kinetics of acidification. The hydrolysis of glucono-'lactone (GdL) provides a slow pH drop that allows for stepwise triggering of peptide components into essentially self-sorted nanostructures based on subtle pKa differences, whereas HCl addition leads to a rapid formation of mixed components within a nanostructure. Using 1H NMR spectroscopy and fiber X-ray diffraction, we determine the conditions and peptide mixtures that favor self-sorting or intimate comixing. Photophysical investigations in the solution phase provide insight into the correlation of energy-transport processes occurring within the assemblies to the structural organization of the π-systems.
Original languageEnglish
Pages (from-to)8685-8692
Number of pages8
JournalJournal of the American Chemical Society
Volume139
Issue number25
Early online date16 Jun 2017
DOIs
Publication statusPublished - 28 Jun 2017

Keywords

  • Nanostructures
  • Supramolecular structures and assemblies
  • Peptides and proteins
  • Absorption
  • Hydrogels

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