All-Atom Molecular Dynamics Simulations of Peptide Amphiphile Assemblies That Spontaneously Form Twisted and Helical Ribbon Structures

Cheng Tsung Lai, Nathaniel L. Rosi, George C Schatz

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

Self-assembly of peptide amphiphiles (PAs) has been an active research area as the assemblies can be programmed into variously shaped nanostructures. Although cylindrical micelles are common structures, gold-binding peptide conjugates can self-assemble into chiral nanofibers with single or double helices. When gold nanoparticles bind to the helices, the resulting chiral nanoparticle assemblies have a collective plasmonic circular dichroism signal that can serve as nanoscale circular polarizers or chiroptical sensors. A better atomic-level understanding of the factors which lead to helical PA assemblies is therefore of significant importance. In this study we show that all-atom molecular dynamics simulations can describe the spontaneous structural transformation from a planar assembly of PAs to a twisted assembly or to a helical ribbon. The twist angle and the helical diameter calculated from the simulations closely match the experimental results, with the oxidation of a single Met residue in each PA leading to a change from bilayer to monolayer assemblies with significantly different ribbon properties. A secondary structure analysis shows how a combination of β-sheet formation near the hydrophobic core of the micelle and PPII structures from proline-rich C-terminus regions favors helix formation. The simulations presented here demonstrate the capability of predicting self-assembly in chiral structures, protocols that can easily be applied to the assembly of other amphiphilic molecules.

Original languageEnglish
Pages (from-to)2170-2174
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume8
Issue number10
DOIs
Publication statusPublished - May 18 2017

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Amphiphiles
assemblies
Peptides
ribbons
peptides
Molecular dynamics
molecular dynamics
Atoms
helices
Computer simulation
assembly
atoms
simulation
self assembly
micelles
Micelles
gold
Gold
Self assembly
nanoparticles

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

All-Atom Molecular Dynamics Simulations of Peptide Amphiphile Assemblies That Spontaneously Form Twisted and Helical Ribbon Structures. / Lai, Cheng Tsung; Rosi, Nathaniel L.; Schatz, George C.

In: Journal of Physical Chemistry Letters, Vol. 8, No. 10, 18.05.2017, p. 2170-2174.

Research output: Contribution to journalArticle

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