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@ARTICLE{Fischer:890360,
author = {Fischer, Jennifer and Radulescu, Aurel and Falus, Peter and
Richter, Dieter and Biehl, Ralf},
title = {{S}tructure and {D}ynamics of {R}ibonuclease {A} during
{T}hermal {U}nfolding: {T}he {F}ailure of the {Z}imm
{M}odel},
journal = {The journal of physical chemistry / B},
volume = {125},
number = {3},
issn = {1520-5207},
address = {Washington, DC},
publisher = {Soc.},
reportid = {FZJ-2021-00905},
pages = {780 - 788},
year = {2021},
abstract = {Disordered regions as found in intrinsically disordered
proteins (IDP) or during protein folding define response
time to stimuli and protein folding times. Neutron spin-echo
spectroscopy is a powerful tool to directly access the
collective motions of the unfolded chain to enlighten the
physical origin of basic conformational relaxation. During
the thermal unfolding of native ribonuclease A, we examine
the structure and dynamics of the disordered state within a
two-state transition model using polymer models, including
internal friction, to describe the chain dynamics. The
presence of four disulfide bonds alters the disordered
configuration to a more compact configuration compared to a
Gaussian chain that is defined by the additional links, as
demonstrated by coarse-grained simulation. The dynamics of
the disordered chain is described by Zimm dynamics with
internal friction (ZIF) between neighboring amino acids.
Relaxation times are dominated by mode-independent internal
friction. Internal friction relaxation times show an
Arrhenius-like behavior with an activation energy of 33
kJ/mol. The Zimm dynamics is dominated by internal friction
and suggest that the characteristic motions correspond to
overdamped elastic modes similar to the motions observed for
folded proteins but within a pool of disordered
configurations spanning the configurational space. For IDP,
internal friction dominates while solvent friction and
hydrodynamic interactions are smaller corrections.},
cin = {JCNS-FRM-II / MLZ / JCNS-1 / JCNS-2 / JCNS-4},
ddc = {530},
cid = {I:(DE-Juel1)JCNS-FRM-II-20110218 / I:(DE-588b)4597118-3 /
I:(DE-Juel1)JCNS-1-20110106 / I:(DE-Juel1)JCNS-2-20110106 /
I:(DE-Juel1)JCNS-4-20201012},
pnm = {6G4 - Jülich Centre for Neutron Research (JCNS) (FZJ)
(POF4-6G4)},
pid = {G:(DE-HGF)POF4-6G4},
experiment = {EXP:(DE-MLZ)KWS2-20140101 /
EXP:(DE-H253)DORISIII(machine)-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {33470118},
UT = {WOS:000614308000009},
doi = {10.1021/acs.jpcb.0c09476},
url = {https://juser.fz-juelich.de/record/890360},
}