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@ARTICLE{Zheng:201205,
author = {Zheng, Wenwei and Vargiu, Attlio Vittorio and Rohrdanz,
Mary A. and Carloni, Paolo and Clementi, Cecilia},
title = {{M}olecular recognition of {DNA} by ligands: {R}oughness
and complexity of the free energy profile},
journal = {The journal of chemical physics},
volume = {139},
number = {14},
issn = {0021-9606},
address = {Melville, NY},
publisher = {American Institute of Physics},
reportid = {FZJ-2015-03510},
pages = {145102 -},
year = {2013},
abstract = {Understanding the molecular mechanism by which probes and
chemotherapeutic agents bind to nucleic acids is a
fundamental issue in modern drug design. From a
computational perspective, valuable insights are gained by
the estimation of free energy landscapes as a function of
some collective variables (CVs), which are associated with
the molecular recognition event. Unfortunately the choice of
CVs is highly non-trivial because of DNA's high flexibility
and the presence of multiple association-dissociation events
at different locations and/or sliding within the grooves.
Here we have applied a modified version of Locally-Scaled
Diffusion Map (LSDMap), a nonlinear dimensionality reduction
technique for decoupling multiple-timescale dynamics in
macromolecular systems, to a metadynamics-based free energy
landscape calculated using a set of intuitive CVs. We
investigated the binding of the organic drug anthramycin to
a DNA 14-mer duplex. By performing an extensive set of
metadynamics simulations, we observed sliding of anthramycin
along the full-length DNA minor groove, as well as several
detachments from multiple sites, including the one
identified by X-ray crystallography. As in the case of
equilibrium processes, the LSDMap analysis is able to
extract the most relevant collective motions, which are
associated with the slow processes within the system, i.e.,
ligand diffusion along the minor groove and dissociation
from it. Thus, LSDMap in combination with metadynamics (and
possibly every equivalent method) emerges as a powerful
method to describe the energetics of ligand binding to DNA
without resorting to intuitive ad hoc reaction coordinates.},
cin = {GRS / IAS-5},
ddc = {540},
cid = {I:(DE-Juel1)GRS-20100316 / I:(DE-Juel1)IAS-5-20120330},
pnm = {899 - ohne Topic (POF2-899)},
pid = {G:(DE-HGF)POF2-899},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000325780800055},
pubmed = {pmid:24116648},
doi = {10.1063/1.4824106},
url = {https://juser.fz-juelich.de/record/201205},
}