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@ARTICLE{Hanke:838494,
author = {Hanke, Christian and Gohlke, Holger},
title = {{T}ertiary {I}nteractions in the {U}nbound
{G}uanine-{S}ensing {R}iboswitch {F}ocus {F}unctional
{C}onformational {V}ariability on the {B}inding {S}ite},
journal = {Journal of chemical information and modeling},
volume = {57},
number = {11},
issn = {0095-2338},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2017-07091},
pages = {2822–2832},
year = {2017},
abstract = {Riboswitches are genetic regulatory elements mainly found
in bacteria, which regulate gene expression based on the
availability of a ligand. Purine-sensing riboswitches,
including the guanine-sensing riboswitch (Gsw), possess
tertiary interactions connecting the L2 and L3 loops. These
interactions are important for ligand binding to the
aptamer. However, atomic-level structural knowledge about
the unbound state and how the tertiary interactions
influence the conformational heterogeneity of the aptamer is
still scarce. We performed replica exchange molecular
dynamics simulations of the aptamer domain of wild type Gsw
and a G37A/C61U mutant, which exhibits destabilized tertiary
interactions, at different Mg2+ concentrations with an
aggregate simulation time of ~16 µs, and subsequently
obtained free energy landscapes. Our data provide evidence
that suggests that the unbound state of wild type Gsw is
conformationally rather homogeneous from a global view
point, yet the ligand binding site shows functionally
necessary mobility required for ligand binding. For the
mutant, the data suggest a heterogeneous ensemble, in
particular without Mg2+. Hence, the tertiary interactions
focus functional conformational variability on the binding
site region of wild type Gsw. Our data allows speculating
that already the weakening of the tertiary interactions by
two hydrogen bonds shifts the kinetics of folding from
downhill folding without traps or intermediate states for
wild type Gsw to a folding including intermediates and
misfolded structures for the mutant. A slowed-down folding
of the aptamer might favor a decision during transcriptional
regulation for the off-path, even if the ligand binds.},
cin = {JSC / ICS-6 / NIC},
ddc = {540},
cid = {I:(DE-Juel1)JSC-20090406 / I:(DE-Juel1)ICS-6-20110106 /
I:(DE-Juel1)NIC-20090406},
pnm = {551 - Functional Macromolecules and Complexes (POF3-551) /
511 - Computational Science and Mathematical Methods
(POF3-511) / Impact of conformational heterogeneity of
riboswitches on gene regulation $(hdd08_20111101)$},
pid = {G:(DE-HGF)POF3-551 / G:(DE-HGF)POF3-511 /
$G:(DE-Juel1)hdd08_20111101$},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:29019403},
UT = {WOS:000416614900019},
doi = {10.1021/acs.jcim.7b00567},
url = {https://juser.fz-juelich.de/record/838494},
}