Related papers: Revisiting the Electrified Pt(111)/Water Interface…
Liquid water is fundamentally important, and its accurate computer simulation has been the driving force for myriad methodological developments. Ab initio molecular dynamics with forces obtained from density functional theory (DFT) is now a…
Why kinetically stable oil droplets in water spontaneously acquire a negative charge remains one of the most vigorously debated questions in interfacial science. Here, we combine neural-network based deep potential molecular dynamics with a…
Semipermeable silica membranes are attractive as protective coatings for metal electrocatalysts such as platinum but their impact on the catalytic properties has not been fully understood. Here, we develop a first principles formalism to…
The distribution of ions at the air/water interface plays a decisive role in many natural processes. It is generally understood that polarizable ions with low charge density are surface-active, implying they sit on top of the water surface.…
Ab initio techniques have revolutionised the way in which theory can help practitioners to explore critical mechanisms that govern reactions or properties, and to develop new strategies for materials discovery and design. Yet, their…
Site density functional theory (SDFT) provides a rigorous framework for statistical mechanics analysis of inhomogeneous molecular liquids. The key defining feature of these systems is the presence of two very distinct interactions scales…
We present a modification to our recently published SAFT-based classical density functional theory for water. We have recently developed and tested a functional for the averaged radial distribution function at contact of the hard-sphere…
The differential capacitance comprises the most relevant thermodynamic information about an electrochemical system. Classical approaches to describe electrochemical capacitance have difficulties to combine the treatment of the ionic…
We consider a model fluid with long-ranged, dispersion interparticle potentials confined between competing parallel walls. One wall is solvophilic and would be completely wet at bulk liquid-gas coexistence while the other is solvophobic and…
To further develop accurate and large-scale simulations of electrochemical interfaces, we propose a unified explicit electric potential framework to simultaneously predict atomic forces and electron density distributions. The framework…
In this work, the tetrahydrofuran (THF) hydrate-water interfacial free energy is determined at $500\,\text{bar}$, at one point of the univariant two-phase coexistence line of the THF hydrate, by molecular dynamics simulation. The Mold…
Hydrophobic solid-water interfaces underpin processes in nanofluidics, electrochemistry, and energy technologies. Microscopic insights into these systems are often inferred from our understanding of the air-water interface, which is assumed…
Three dimensional implementations of liquid state theories offer an efficient alternative to computer simulations for the atomic-level description of aqueous solutions in complex environments. In this context, we present a (classical)…
Simulating electrified metal/water interfaces with explicit solvent under constant potential is essential for understanding electrochemical processes, yet remains prohibitively expensive with ab initio methods. We present TRECI, a…
Hydrogenation of amorphous silicon (a-Si:H) is critical for reducing defect densities, passivating mid-gap states and surfaces, and improving photoconductivity in silicon-based electro-optical devices. Modelling the atomic scale structure…
Understanding ion adsorption at electrified metal-electrolyte interfaces is essential for accurate modeling of electrochemical systems. Here, we systematically investigate the free energy profiles of Na$^+$, Cl$^-$, and F$^-$ ions at the…
The structure of the double-layer formed at the surface of carbon electrodes is governed by the interactions between the electrode and the electrolyte species. However, carbon is notoriously difficult to simulate accurately, even with…
Recent advances in continuum embedding models have enabled the incorporation of solvent and electrolyte effects into density functional theory (DFT) simulations of material surfaces, significantly benefiting electrochemistry, catalysis, and…
Far from being conclusively understood, the reactive interaction of water with rutile does still present a challenge to atomistic modelling techniques rooted on quantum mechanics. We show that static geometries of stoichiometric…
Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…