Related papers: Reactions at surfaces studied by ab initio dynamic…
Recent experimental results about the formation of molecular hydrogen on astrophysically relevant surfaces under conditions close to those encountered in the interstellar medium are analyzed using rate equations. The parameters of the rate…
Obtaining the free energies of condensed phase chemical reactions remains computationally prohibitive for high-level quantum mechanical methods. We introduce a hierarchical machine learning framework that bridges this gap by distilling…
We study the dissociative adsorption of methane at the surface of graphene. Free energy profiles, which include activation energies for different steps of the reaction, are computed from constrained ab initio molecular dynamics. At 300 K,…
Solid-On-Solid (SOS) computer simulations are employed to investigate the sublimation of surfaces. We distinguish three sublimation regimes: layer-by-layer sublimation, free step flow and hindered step flow. The sublimation regime is…
Adsorption and dissociation of hydrocarbons on metallic surfaces represent crucial steps to carburization of metal. Here, we use density functional theory total energy calculations with the climbing-image nudged elastic band method to…
We present a general computational scheme based on molecular dynamics (m.d.) simulation for calculating the chemical potential of adsorbed molecules in thermal equilibrium on the surface of a material. The scheme is based on the calculation…
The potential energy surface (PES) of dissociative adsorption of H_2 on Pd(100) is investigated using density functional theory and the full-potential linear augmented plane wave (FP-LAPW) method. Several dissociation pathways are…
Atomistic simulations using accurate energy functions can provide molecular-level insight into functional motions of molecules in the gas- and in the condensed phase. Together with recently developed and currently pursued efforts in…
We study the dynamics of simple reactions where the chemical species are confined on a general, time-modulated surface, and subjected to externally-imposed stirring. The study of these inhomogeneous effects requires a model based on a…
We study the opportunities for parallelism for the simulation of surface reactions. We introduce the concept of a partition and we give new simulation methods based on Cellular Automaton using partitions. We elaborate on the advantages and…
Understanding of the complex behavior of particles at surfaces requires detailed knowledge of both macroscopic and microscopic processes that take place; also certain processes depend critically on temperature and gas pressure. To link…
Understanding surface reactivity is crucial in many fields, going from heterogeneous catalysis to materials oxidation and corrosion. In order to decipher the surface reactions of ZrB2 exposed to the harsh environment of aerospace…
In the standard treatment of heterogeneous nucleation on a surface, the energy of the surface is assumed to be homogeneous. Often its value is obtained from some macroscopic measurement. We ask the question what happens if we consider the…
The pervasive phenomenon of friction has been studied at the nanoscale by controlled manipulation of single atoms and molecules, which permitted a precise determination of the static friction force necessary to initiate motion. However,…
Diffusion-mediated surface phenomena are crucial for human life and industry, with examples ranging from oxygen capture by lung alveolar surface to heterogeneous catalysis, gene regulation, membrane permeation and filtration processes.…
A general approach to calculate the diabatic surfaces for electron-transfer reactions is presented, based on first-principles molecular dynamics of the active centers and their surrounding medium. The excitation energy corresponding to the…
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…
Relations between the thermodynamics and dynamics of supercooled liquids approaching a glass transition have been proposed over many years. The potential energy surface of model liquids has been increasingly studied since it provides a…
The reaction dynamics for the H + HeH$^+$ $\rightarrow$ He + H$_2^+$ reaction in its electronic ground state is investigated using two different representations of the potential energy surface (PES). The first uses a combined kernel and…
Reaction probabilities as a function of total angular momentum and the resulting reaction cross-sections for the collision of open shell S($^1$D) atoms with para-hydrogen have been calculated in the kinetic energy range 0.09--10 meV (1--120…