相关论文: Non-adiabatic effects during the dissociative adso…
The measured low initial sticking probability of oxygen molecules at the Al(111) surface that had puzzled the field for many years was recently explained in a non-adiabatic picture invoking spin-selection rules [J. Behler et al., Phys. Rev.…
Electronic friction and the ensuing nonadiabatic energy loss play an important role in chemical reaction dynamics at metal surfaces. Using molecular dynamics with electronic friction evaluated on-the-fly from Density Functional Theory, we…
A high-dimensional potential energy surface (PES) for CO interaction with the Au(111) surface is developed using a machine-learning algorithm. Including both molecular and surface coordinates, this PES enables the simulation of the recent…
Accurate description of nonadiabatic dynamics of molecules at metal surfaces involving electron transfer has been a longstanding challenge for theory. Here, we tackle this problem by first constructing high-dimensional neural network…
Non-adiabatic effects play an important role in many chemical processes. In order to study the underlying non-adiabatic potential-energy surfaces (PESs), we present a locally-constrained density-functional theory approach, which enables us…
We have investigated the quantum dynamics of O2 dissociative adsorption on a Ag(111) surface. We performed the calculations with a Hamiltonian where the O2 translational motion is perpendicular to the surface and for O2 vibrational energy.…
By performing first-principles molecular dynamics calculations, we systematically simulate the adsorption behavior of oxygen molecules on the clean and strained Pb(111) surfaces. The obtained molecular adsorption precursor state, and the…
Experimental observations of multi-quantum relaxation of highly vibrationally excited NO scattering from Au(111) are a benchmark for the breakdown of Born-Oppenheimer approximation in molecule-surface systems. This remarkable vibrational…
In this work we investigate the dissociation of CO$_2$ on Cu(110) by performing density functional theory calculations using the vdW-DF2 exchange-correlation functional, with a potential energy surface parameterized using artificial neural…
Recently, spin selection rules have been invoked to explain the discrepancy between measured and calculated adsorption probabilities of molecular oxygen reacting with Al(111). In this work, we inspect the impact of nonadiabatic spin…
Dissociative chemisorption is a key process in hydrogen-metal surface chemistry, where nonadiabatic effects due to low-lying electron-hole-pair excitations may affect reaction outcomes. Molecular dynamics with electronic friction…
A most basic and puzzling enigma in surface science is the description of the dissociative adsorption of O2 at the (111) surface of Al. Already for the sticking curve alone, the disagreement between experiment and results of…
The adsorption and dissociation of O$_{2}$ molecules at the Be(0001) surface is studied by using density-functional theory within the generalized gradient approximation and a supercell approach. The physi- and chemisorbed molecular…
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…
To help provide insight into the remarkable catalytic behavior of the oxygen/silver system for heterogeneous oxidation reactions, purely sub-surface oxygen, and structures involving both on-surface and sub-surface oxygen, as well as…
Nonadiabatic effects that arise from the concerted motion of electrons and atoms at comparable energy and time scales are omnipresent in thermal and light-driven chemistry at metal surfaces. Excited (hot) electrons can measurably affect…
The adsorption of atomic oxygen and its inclusion into subsurface sites on Ag(210) and Ag(410) surfaces have been investigated using density functional theory. We find that--in the absence of adatoms on the first metal layer--subsurface…
A new methodology of simulating nonadiabatic dynamics using frozen-width Gaussian wavepackets within the moving crude adiabatic representation with the on-the-fly evaluation of electronic structure is presented. The main feature of the new…
Due to the improvement of computer power and the development of efficient algorithms it is now possible to combine high-dimensional quantum dynamical calculations of the dissociative adsorption of molecular beams with reliable ab-initio…
The adsorption and dissociation of nitrogen molecule on Fe(111) surface is studied by density functional theory calculations. The simulation results show that the molecule needs to acquire parallel orientation with respect to the surface…