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@ARTICLE{Owen:823866,
author = {Owen, Michael C. and Strodel, Birgit and Csizmadia, Imre G.
and Viskolcz, Béla},
title = {{R}adical {F}ormation {I}nitiates {S}olvent-{D}ependent
{U}nfolding and β-{S}heet {F}ormation in a {M}odel
{H}elical {P}eptide},
journal = {The journal of physical chemistry / B},
volume = {120},
number = {22},
issn = {1520-5207},
address = {Washington, DC},
publisher = {Soc.},
reportid = {FZJ-2016-06506},
pages = {4878 - 4889},
year = {2016},
abstract = {We examined the effects of Cα-centered radical formation
on the stability of a model helical peptide,
N-Ac-KK(AL)10KK-NH2. Three, 100 ns molecular dynamics
simulations using the OPLS-AA force field were carried out
on each α-helical peptide in six distinct binary TIP4P
water/2,2,2-trifluoroethanol (TFE) mixtures. The α-helicity
was at a maximum in $20\%$ TFE, which was inversely
proportional to the number of H-bonds between water
molecules and the peptide backbone. The radial distribution
of TFE around the peptide backbone was highest in $20\%$
TFE, which enhanced helix stability. The Cα-centered
radical initiated the formation of a turn within 5 ns, which
was a smaller kink at high TFE concentrations, and a loop at
lower TFE concentrations. The highest helicity of the
peptide radical was measured in $100\%$ TFE. The formation
of hydrogen bonds between the peptide backbone and water
destabilized the helix, whereas the clustering of TFE
molecules around the radical center stabilized the helix.
Following radical termination, the once helical structure
converted to a β-sheet rich state in $100\%$ water only,
and this transition did not occur in the nonradical control
peptide. This study gives evidence on how the formation of
peptide radicals can initiate α-helical to β-sheet
transitions under oxidative stress conditions.},
cin = {ICS-6},
ddc = {530},
cid = {I:(DE-Juel1)ICS-6-20110106},
pnm = {553 - Physical Basis of Diseases (POF3-553)},
pid = {G:(DE-HGF)POF3-553},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000377841200002},
pubmed = {pmid:27169334},
doi = {10.1021/acs.jpcb.6b00174},
url = {https://juser.fz-juelich.de/record/823866},
}