@sfb1313-puma

Electronic screening using a virtual Thomas--Fermi fluid for predicting wetting and phase transitions of ionic liquids at metal surfaces

, , , and . Nature Materials, (Nov 11, 2021)
DOI: 10.1038/s41563-021-01121-0

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 $łambda$. 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.

Links and resources

Tags

community