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@ARTICLE{Bruch:1023017,
author = {Bruch, Nils and Binninger, Tobias and Huang, Jun and
Eikerling, Michael},
title = {{I}ncorporating {E}lectrolyte {C}orrelation {E}ffects into
{V}ariational {M}odels of {E}lectrochemical {I}nterfaces},
journal = {The journal of physical chemistry letters},
volume = {15},
number = {7},
issn = {1948-7185},
address = {Washington, DC},
publisher = {ACS},
reportid = {FZJ-2024-01600},
pages = {2015 - 2022},
year = {2024},
abstract = {We propose a way for obtaining a classical free energy
density functional for electrolytes based on a
first-principle many-body partition function. Via a one-loop
expansion, we include coulombic correlations beyond the
conventional mean-field approximation. To examine
electrochemical interfaces, we integrate the electrolyte
free energy functional into a hybrid quantum-classical
model. This scheme self-consistently couples electronic,
ionic, and solvent degrees of freedom and incorporates
electrolyte correlation effects. The derived free energy
functional causes a correlation-induced enhancement in
interfacial counterion density and leads to an overall
increase in capacitance. This effect is partially
compensated by a reduction of the dielectric permittivity of
interfacial water. At larger surface charge densities, ion
crowding at the interface stifles these correlation effects.
While scientifically intriguing already at planar
interfaces, we anticipate these correlation effects to play
an essential role for electrolytes in nanoconfinement.},
cin = {IEK-13},
ddc = {530},
cid = {I:(DE-Juel1)IEK-13-20190226},
pnm = {1212 - Materials and Interfaces (POF4-121)},
pid = {G:(DE-HGF)POF4-1212},
typ = {PUB:(DE-HGF)16},
pubmed = {38349906},
UT = {WOS:001167244700001},
doi = {10.1021/acs.jpclett.3c03295},
url = {https://juser.fz-juelich.de/record/1023017},
}