相关论文: Ab initio surface chemistry with chemical accuracy
Although perovskite oxides hold promise in applications ranging from solid oxide fuel cells to catalysts, their surface chemistry is poorly understood at the molecular level. Here we follow the formation of the first monolayer of water at…
Density functional theory (DFT) is widely used in surface science, but gives poor accuracy for oxide surface processes, while high-level quantum chemistry methods are hard to apply without losing basis-set quality. We argue that quantum…
Interactions between molecules and electrode surfaces play a key role in electrochemical processes and are a subject of extensive research, both experimental and theoretical. In this manuscript, we address the water dissociation reaction on…
Accurate thermochemical data with sub-chemical accuracy (within 1 kcal mol$^{-1}$ of the empirical ground truth) are essential for advancing computational chemistry methods. However, existing datasets that reach this level of accuracy…
Surfaces of metal oxides at working conditions are usually electrified due to the acid-base chemistry. The charged interface compensated with counterions forms the so-called electric double layer. The coupling of surface chemistry and…
In order to obtain a comprehensive understanding of both thermodynamics and kinetics of water dissociation on TiO2, the reactions between liquid water and perfect and defective rutile TiO2 (110) surfaces were investigated using ab initio…
We propose a generalisation of molecular density functional theory to describe inhomogeneous solvent mixture, with the objective of modelling electrolytic solutions. Two electrolytic models are presented, both within the HNC approximation.…
Water/solid interfaces are relevant to a broad range of physicochemical phenomena and technological processes such as corrosion, lubrication, heterogeneous catalysis and electrochemistry. Although many fields have contributed to rapid…
Clay minerals are ubiquitous in nature, and the manner in which they interact with their surroundings has important industrial and environmental implications. Consequently, a molecular-level understanding of the adsorption of molecules on…
Water adsorption on silicate surfaces is a critical yet poorly understood process relevant to, e.g., mineral weathering and cement hydration. This study investigates the structure of water overlayers on a model calcium silicate, the…
The contact angle of a liquid droplet on a solid surface is a direct measure of fundamental atomic-scale forces acting between liquid molecules and the solid surface. In this work, the validity is assessed of a simple equation, which…
Computing accurate rate constants for catalytic events occurring at the surface of a given material represents a challenging task with multiple potential applications in chemistry. To address this question, we propose an approach based on a…
Computationally efficient and accurate quantum mechanical approximations to solve the many-electron Schr\"odinger equation are at the heart of computational materials science. In that respect the coupled cluster hierarchy of methods plays a…
Quantum-mechanical methods are widely used for understanding molecular interactions throughout biology, chemistry, and materials science. Quantum diffusion Monte Carlo (DMC) and coupled cluster with single, double, and perturbative triple…
Water and silicon are chemically dissimilar substances with common physical properties. Their liquids display a temperature of maximum density, increased diffusivity on compression, they form tetrahedral crystals and tetrahedral amorphous…
We study the surface tension of electrolyte solutions at the air/water and oil/water interfaces. Employing field-theoretical methods and considering short-range interactions of anions with the surface, we expand the Helmholtz free energy to…
It remains a prime question of how to describe the optical properties of large molecular clusters accurately. Quantum chemical methods capture essential electronic details but are infeasible for entire clusters, while optical simulations…
Closed-form, analytical approximations for electrostatic properties of molecules are of unique value, as these can provide computational speed, versatility, and physical insight. Here, we derive a simple, closed-form formula for the…
The estimation of the surface tension of water is theoretically dealt on the basis of the dipole molecular model. It is known that the experimentally determined surface tension of freshly exposed surface has a higher value than the nominal…
Recent disagreement between state-of-the-art quantum chemical methods, coupled cluster with single, double and perturbative triples excitations and fixed-node diffusion Monte Carlo, calls for systematic examination of possible sources of…