1. Cyanine Dye Coupling Mediates Self‐assembly of a pH Sensitive Peptide into Novel 3D Architectures
- Author
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Rita Fernandes, Suvrat Chowdhary, Natalia Mikula, Noureldin Saleh, Katerina Kanevche, Hans v. Berlepsch, Naoki Hosogi, Joachim Heberle, Marcus Weber, Christoph Böttcher, and Beate Koksch
- Subjects
Chromophore Assembly ,Cyanines ,General Chemistry ,General Medicine ,Carbocyanines ,Hydrogen-Ion Concentration ,Catalysis ,Electron Microscopy ,500 Naturwissenschaften und Mathematik::540 Chemie::540 Chemie und zugeordnete Wissenschaften ,Coloring Agents ,Peptides ,De Novo Peptide ,H-Aggregates - Abstract
Synthetic multichromophore systems are of great importance in artificial light harvesting devices, organic optoelectronics, tumor imaging and therapy. Here, we introduce a promising strategy for the construction of self-assembled peptide templated dye stacks based on coupling of a de novo designed pH sensitive peptide with a cyanine dye Cy5 at its N-terminus. Microscopic techniques, in particular cryogenic TEM (cryo-TEM) and cryo-electron tomography technique (cryo-ET), reveal two types of highly ordered three-dimensional assembly structures on the micrometer scale. Unbranched compact layered rods are observed at pH 7.4 and two-dimensional membrane-like assemblies at pH 3.4, both species displaying spectral features of H-aggregates. Molecular dynamics simulations reveal that the coupling of Cy5 moieties promotes the formation of both ultrastructures, whereas the protonation states of acidic and basic amino acid side chains dictates their ultimate three-dimensional organization.
- Published
- 2022
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