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@ARTICLE{Dapp:139147,
author = {Dapp, Wolfgang and Müser, Martin},
title = {{T}owards time-dependent, non-equilibrium charge-transfer
force fields},
journal = {The European physical journal / B},
volume = {86},
number = {7},
issn = {1434-6036},
address = {Berlin},
publisher = {Springer},
reportid = {FZJ-2013-05154},
pages = {337},
year = {2013},
abstract = {Force fields uniquely assign interatomic forces for a given
set of atomic coordinates. The underlying assumption is that
electrons are in their quantum-mechanical ground state or in
thermal equilibrium. However, there is an abundance of cases
where this is unjustified because the system is only locally
in equilibrium. In particular, the fractional charges of
atoms, clusters, or solids tend to not only depend on atomic
positions but also on how the system reached its state. For
example, the charge of an isolated solid -- and thus the
forces between atoms in that solid -- usually depends on the
counterbody with which it has last formed contact.
Similarly, the charge of an atom, resulting from the
dissociation of a molecule, can differ for different
solvents in which the dissociation took place. In this paper
we demonstrate that such charge-transfer history effects can
be accounted for by assigning discrete oxidation states to
atoms. With our method, an atom can donate an integer charge
to another, nearby atom to change its oxidation state as in
a redox reaction. In addition to integer charges, atoms can
exchange "partial charges" which are determined with the
split charge equilibration method.},
cin = {JSC},
ddc = {530},
cid = {I:(DE-Juel1)JSC-20090406},
pnm = {411 - Computational Science and Mathematical Methods
(POF2-411)},
pid = {G:(DE-HGF)POF2-411},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000333400700004},
doi = {10.1140/epjb/e2013-40047-x},
url = {https://juser.fz-juelich.de/record/139147},
}