Structural and Spectroscopic Properties of Assemblies of Self-Replicating Peptide Macrocycles
| Autor: | Siewert J. Marrink, Anna S. Bondarenko, Mathieu Surin, Thomas L. C. Jansen, Gaël Schaeffer, Yigit Altay, Julien Idé, Sijbren Otto, David Beljonne, Pim W. J. M. Frederix |
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| Přispěvatelé: | Molecular Dynamics, Synthetic Organic Chemistry, Theory of Condensed Matter |
| Jazyk: | angličtina |
| Rok vydání: | 2017 |
| Předmět: |
DYNAMICS
Circular dichroism spectroscopy Absorption spectroscopy PROTEINS Supramolecular chemistry General Physics and Astronomy Infrared spectroscopy Molecular Dynamics Simulation 010402 general chemistry 01 natural sciences self-replication Article Molecular dynamics 0103 physical sciences nanostructures IMPLEMENTATION Molecule General Materials Science AMPHIPHILES Protein secondary structure chemistry.chemical_classification MOLECULAR SIMULATION 010304 chemical physics Circular Dichroism General Engineering WATER MODELS self-assembly DRIVEN simulation molecular dynamics 0104 chemical sciences Supramolecular polymers GROMOS FORCE-FIELD SUPRAMOLECULAR POLYMERS Crystallography chemistry Chemical physics peptides AMYLOID FIBRIL |
| Zdroj: | ACS Nano Acs Nano, 11(8), 7858-7868. AMER CHEMICAL SOC |
| ISSN: | 1936-086X 1936-0851 |
| Popis: | Self-replication at the molecular level is often seen as essential to the early origins of life. Recently a mechanism of self-replication has been discovered in which replicator self-assembly drives the process. We have studied one of the examples of such self-assembling self-replicating molecules to a high level of structural detail using a combination of computational and spectroscopic techniques. Molecular Dynamics simulations of self-assembled stacks of peptide-derived replicators provide insights into the structural characteristics of the system and serve as the basis for semiempirical calculations of the UV-vis, circular dichroism (CD) and infrared (IR) absorption spectra that reflect the chiral organization and peptide secondary structure of the stacks. Two proposed structural models are tested by comparing calculated spectra to experimental data from electron microscopy, CD and IR spectroscopy, resulting in a better insight into the specific supramolecular interactions that lead to self-replication. Specifically, we find a cooperative self-assembly process in which β-sheet formation leads to well-organized structures, while also the aromatic core of the macrocycles plays an important role in the stability of the resulting fibers. |
| Databáze: | OpenAIRE |
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