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@ARTICLE{Zhang:201297,
author = {Zhang, C. and Knyazev, D. G. and Vereshaga, Y. A. and
Ippoliti, E. and Nguyen, T. H. and Carloni, P. and Pohl, P.},
title = {{W}ater at hydrophobic interfaces delays proton
surface-to-bulk transfer and provides a pathway for lateral
proton diffusion},
journal = {Proceedings of the National Academy of Sciences of the
United States of America},
volume = {109},
number = {25},
issn = {1091-6490},
address = {Washington, DC},
publisher = {National Acad. of Sciences},
reportid = {FZJ-2015-03602},
pages = {9744 - 9749},
year = {2012},
abstract = {Fast lateral proton migration along membranes is of vital
importance for cellular energy homeostasis and various
proton-coupled transport processes. It can only occur if
attractive forces keep the proton at the interface. How to
reconcile this high affinity to the membrane surface with
high proton mobility is unclear. Here, we tested whether a
minimalistic model interface between an apolar hydrophobic
phase (n-decane) and an aqueous phase mimics the biological
pathway for lateral proton migration. The observed diffusion
span, on the order of tens of micrometers, and the high
proton mobility were both similar to the values previously
reported for lipid bilayers. Extensive ab initio simulations
on the same water∕n-decane interface reproduced the
experimentally derived free energy barrier for the excess
proton. The free energy profile adopts the shape of a well
at the interface, having a width oftwo water molecules and a
depth of 6 +/- 2RT. The hydroniums in direct contact with
n-decane have a reduced mobility. However, the hydroniums in
the second layer of water molecules are mobile. Their in
silico diffusion coefficient matches that derived from our
in vitro experiments, 5.7 +/- 0.7 × $10^−5$ $cm^2$
$s^−1.$ Conceivably, these are the protons that allow for
fast diffusion along biological membranes.},
cin = {GRS / IAS-5},
ddc = {000},
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:000306061400025},
pubmed = {pmid:22675120},
doi = {10.1073/pnas.1121227109},
url = {https://juser.fz-juelich.de/record/201297},
}