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@ARTICLE{Casasnovas:829377,
author = {Casasnovas, Rodrigo and Limongelli, Vittorio and Tiwary,
Pratyush and Carloni, Paolo and Parrinello, Michele},
title = {{U}nbinding {K}inetics of a p38 {MAP} {K}inase {T}ype {II}
{I}nhibitor from {M}etadynamics {S}imulations},
journal = {Journal of the American Chemical Society},
volume = {139},
number = {13},
issn = {1520-5126},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2017-03090},
pages = {4780 - 4788},
year = {2017},
abstract = {Understanding the structural and energetic requisites of
ligand binding toward its molecular target is of paramount
relevance in drug design. In recent years, atomistic free
energy calculations have proven to be a valid tool to
complement experiments in characterizing the thermodynamic
and kinetic properties of protein/ligand interaction. Here,
we investigate, through a recently developed
metadynamics-based protocol, the unbinding mechanism of an
inhibitor of the pharmacologically relevant target p38 MAP
kinase. We provide a thorough description of the ligand
unbinding pathway identifying the most stable binding mode
and other thermodynamically relevant poses. From our
simulations, we estimated the unbinding rate as koff = 0.020
± 0.011 s–1. This is in good agreement with the
experimental value (koff = 0.14 s–1). Next, we developed a
Markov state model that allowed identifying the
rate-limiting step of the ligand unbinding process. Our
calculations further show that the solvation of the ligand
and that of the active site play crucial roles in the
unbinding process. This study paves the way to
investigations on the unbinding dynamics of more complex p38
inhibitors and other pharmacologically relevant inhibitors
in general, demonstrating that metadynamics can be a
powerful tool in designing new drugs with engineered
binding/unbinding kinetics.},
cin = {IAS-5 / INM-9},
ddc = {540},
cid = {I:(DE-Juel1)IAS-5-20120330 / I:(DE-Juel1)INM-9-20140121},
pnm = {574 - Theory, modelling and simulation (POF3-574)},
pid = {G:(DE-HGF)POF3-574},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000398764000030},
pubmed = {pmid:28290199},
doi = {10.1021/jacs.6b12950},
url = {https://juser.fz-juelich.de/record/829377},
}