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Title: Self-Assembly and Molecular Dynamics of Peptide-Functionalized Polyphenylene Dendrimers

Abstract

The self-assembly mechanism and the associated molecular dynamics are studied for a series of poly-L-lysine-functionalized polyphenylene dendrimer melts as a function of the core size (generation), functionality, and polypeptide length using X-rays, solid-state NMR, calorimetry, and dielectric spectroscopy. A striking dependence of the polyphenylene self-assembly on the poly-L-lysine length is shown. In addition, the type ({alpha}helix/{beta}-sheet) of peptide secondary structure is controlled by the packing restrictions imposed by the polyphenylene core. We show that constrained poly-L-lysines can adopt different secondary structures from their linear analogues. The dynamic investigation revealed significant mobility associated solely with the polypeptide through three processes: a glass transition, a slower process associated with the relaxation of {alpha}-helical segments, and a glassy mode whose origin could be resolved by site-specific solid-state NMR techniques. Solid-state NMR studies further indicated a mobility gradient in going from the rigid peptide backbone to the side chains.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Org.:
Doe - Office Of Science
OSTI Identifier:
930237
Report Number(s):
BNL-80919-2008-JA
TRN: US200822%%1414
DOE Contract Number:  
DE-AC02-98CH10886
Resource Type:
Journal Article
Resource Relation:
Journal Name: Macromolecules; Journal Volume: 39
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; CALORIMETRY; DIELECTRIC MATERIALS; DYNAMICS; FUNCTIONS; GLASS; LENGTH; MOBILITY; NUCLEAR MAGNETIC RESONANCE; ORIGIN; PEPTIDES; POLYPEPTIDES; RELAXATION; SIZE; SPECTROSCOPY; STOWING; national synchrotron light source

Citation Formats

Mondeshki,M., Milhov, G., Graf, R., Spiess, H., Mullen, K., Papadopoulos, P., Gitsas, A., and Floudas, G. Self-Assembly and Molecular Dynamics of Peptide-Functionalized Polyphenylene Dendrimers. United States: N. p., 2006. Web. doi:10.1021/ma0621270.
Mondeshki,M., Milhov, G., Graf, R., Spiess, H., Mullen, K., Papadopoulos, P., Gitsas, A., & Floudas, G. Self-Assembly and Molecular Dynamics of Peptide-Functionalized Polyphenylene Dendrimers. United States. doi:10.1021/ma0621270.
Mondeshki,M., Milhov, G., Graf, R., Spiess, H., Mullen, K., Papadopoulos, P., Gitsas, A., and Floudas, G. Sun . "Self-Assembly and Molecular Dynamics of Peptide-Functionalized Polyphenylene Dendrimers". United States. doi:10.1021/ma0621270.
@article{osti_930237,
title = {Self-Assembly and Molecular Dynamics of Peptide-Functionalized Polyphenylene Dendrimers},
author = {Mondeshki,M. and Milhov, G. and Graf, R. and Spiess, H. and Mullen, K. and Papadopoulos, P. and Gitsas, A. and Floudas, G.},
abstractNote = {The self-assembly mechanism and the associated molecular dynamics are studied for a series of poly-L-lysine-functionalized polyphenylene dendrimer melts as a function of the core size (generation), functionality, and polypeptide length using X-rays, solid-state NMR, calorimetry, and dielectric spectroscopy. A striking dependence of the polyphenylene self-assembly on the poly-L-lysine length is shown. In addition, the type ({alpha}helix/{beta}-sheet) of peptide secondary structure is controlled by the packing restrictions imposed by the polyphenylene core. We show that constrained poly-L-lysines can adopt different secondary structures from their linear analogues. The dynamic investigation revealed significant mobility associated solely with the polypeptide through three processes: a glass transition, a slower process associated with the relaxation of {alpha}-helical segments, and a glassy mode whose origin could be resolved by site-specific solid-state NMR techniques. Solid-state NMR studies further indicated a mobility gradient in going from the rigid peptide backbone to the side chains.},
doi = {10.1021/ma0621270},
journal = {Macromolecules},
number = ,
volume = 39,
place = {United States},
year = {Sun Jan 01 00:00:00 EST 2006},
month = {Sun Jan 01 00:00:00 EST 2006}
}