Of relevance to energy storage, electrochemistry and catalysis, ionic and dipolar liquids display unexpected behaviours---especially in confinement. Beyond adsorption, over-screening and crowding effects, experiments have highlighted novel phenomena, such as unconventional screening and the impact of the electronic nature---metallic versus insulating---of the confining surface. Such behaviours, which challenge existing frameworks, highlight the need for tools to fully embrace the properties of confined liquids. Here we introduce a novel approach that involves electronic screening while capturing molecular aspects of interfacial fluids. Although available strategies consider perfect metal or insulator surfaces, we build on the Thomas--Fermi formalism to develop an effective approach that deals with any imperfect metal between these asymptotes. Our approach describes electrostatic interactions within the metal through a `virtual' Thomas--Fermi fluid of charged particles, whose Debye length sets the screening length $łambda$. We show that this method captures the electrostatic interaction decay and electrochemical behaviour on varying $łambda$. By applying this strategy to an ionic liquid, we unveil a wetting transition on switching from insulating to metallic conditions.
%0 Journal Article
%1 schlaich2021electronic
%A Schlaich, Alexander
%A Jin, Dongliang
%A Bocquet, Lyderic
%A Coasne, Benoit
%D 2021
%J Nature Materials
%K EXC2075 PN1 PN3 curated merged
%R 10.1038/s41563-021-01121-0
%T Electronic screening using a virtual Thomas--Fermi fluid for predicting wetting and phase transitions of ionic liquids at metal surfaces
%U https://doi.org/10.1038/s41563-021-01121-0
%X Of relevance to energy storage, electrochemistry and catalysis, ionic and dipolar liquids display unexpected behaviours---especially in confinement. Beyond adsorption, over-screening and crowding effects, experiments have highlighted novel phenomena, such as unconventional screening and the impact of the electronic nature---metallic versus insulating---of the confining surface. Such behaviours, which challenge existing frameworks, highlight the need for tools to fully embrace the properties of confined liquids. Here we introduce a novel approach that involves electronic screening while capturing molecular aspects of interfacial fluids. Although available strategies consider perfect metal or insulator surfaces, we build on the Thomas--Fermi formalism to develop an effective approach that deals with any imperfect metal between these asymptotes. Our approach describes electrostatic interactions within the metal through a `virtual' Thomas--Fermi fluid of charged particles, whose Debye length sets the screening length $łambda$. We show that this method captures the electrostatic interaction decay and electrochemical behaviour on varying $łambda$. By applying this strategy to an ionic liquid, we unveil a wetting transition on switching from insulating to metallic conditions.
@article{schlaich2021electronic,
abstract = {Of relevance to energy storage, electrochemistry and catalysis, ionic and dipolar liquids display unexpected behaviours---especially in confinement. Beyond adsorption, over-screening and crowding effects, experiments have highlighted novel phenomena, such as unconventional screening and the impact of the electronic nature---metallic versus insulating---of the confining surface. Such behaviours, which challenge existing frameworks, highlight the need for tools to fully embrace the properties of confined liquids. Here we introduce a novel approach that involves electronic screening while capturing molecular aspects of interfacial fluids. Although available strategies consider perfect metal or insulator surfaces, we build on the Thomas--Fermi formalism to develop an effective approach that deals with any imperfect metal between these asymptotes. Our approach describes electrostatic interactions within the metal through a `virtual' Thomas--Fermi fluid of charged particles, whose Debye length sets the screening length $\lambda$. We show that this method captures the electrostatic interaction decay and electrochemical behaviour on varying $\lambda$. By applying this strategy to an ionic liquid, we unveil a wetting transition on switching from insulating to metallic conditions.},
added-at = {2023-06-13T14:35:04.000+0200},
author = {Schlaich, Alexander and Jin, Dongliang and Bocquet, Lyderic and Coasne, Benoit},
biburl = {https://puma.ub.uni-stuttgart.de/bibtex/282ea1ee7ac01a7a3a97f269a77c5d7cf/simtech},
day = 11,
doi = {10.1038/s41563-021-01121-0},
interhash = {65dd8091659a607d40b5e086109ea2b7},
intrahash = {82ea1ee7ac01a7a3a97f269a77c5d7cf},
issn = {1476-4660},
journal = {Nature Materials},
keywords = {EXC2075 PN1 PN3 curated merged},
month = {11},
timestamp = {2023-12-06T08:55:18.000+0100},
title = {Electronic screening using a virtual Thomas--Fermi fluid for predicting wetting and phase transitions of ionic liquids at metal surfaces},
url = {https://doi.org/10.1038/s41563-021-01121-0},
year = 2021
}