Related papers: Reactions at surfaces studied by ab initio dynamic…
Reactions on surfaces play an important role in many technological applications. Since these processes are often rather complex, one tries to understand single steps of these complicated reactions by investigating simpler system. In…
The dissociative adsorption of hydrogen on Pd(100) has been studied by ab initio quantum dynamics and ab initio molecular dynamics calculations. Treating all hydrogen degrees of freedom as dynamical coordinates implies a high dimensionality…
Modeling electronic systems is an important application for quantum computers. In the context of materials science, an important open problem is the computational description of chemical reactions on surfaces. In this work, we outline a…
The molecular energies of chemical systems have been successfully calculated on quantum computers, however, more attention has been paid to the dynamic process of chemical reactions in practical application, especially in catalyst design,…
Oxide-water interfaces govern a wide range of physical and chemical processes fundamental to many fields like catalysis, geochemistry, corrosion, electrochemistry, and sensor technology. Near solid oxide surfaces, water behaves differently…
We performed high-dimensional quantum dynamical calculations of the dissociative adsorption and associative desorption of hydrogen on Cu(111). The potential energy surface (PES) is obtained from density functional theory calculations. Two…
Chemical reactions on metal surfaces are important in various processes such as heterogeneous catalysis and nanostructure growth. At moderate or lower temperatures, these reactions generally follow the minimum energy path and temperature…
We report on a many-electron wavefunction theory study for the reaction energetics of hydrogen dissociation on the Si(100) surface. We demonstrate that quantum chemical wavefunction based methods using periodic boundary conditions can…
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…
We report calculations of the dissociative adsorption of H_2 at Pd (100) covered with 1/4 monolayer of sulfur using quantum dynamics as well as molecular dynamics and taking all six degrees of freedom of the two H atoms fully into account.…
The physical processes at the interface of a low-temperature plasma and a solid are extremely complex. They involve a huge number of elementary processes in the plasma, in the solid as well as charge, momentum and energy transfer across the…
A reliable description of surfaces structures in a reactive environment is crucial to understand materials functions. We present a first-principles theory of replica-exchange grand-canonical-ensemble molecular dynamics (REGC-MD) and apply…
Reactive chemistry of molecular hydrogen at surfaces, notably dissociative sticking and hydrogen evolution, plays a crucial role in energy storage and fuel cells. Theoretical studies can help to decipher underlying mechanisms and reaction…
We propose a machine-learning approach based on Bayesian optimization to build global potential energy surfaces (PES) for reactive molecular systems using feedback from quantum scattering calculations. The method is designed to correct for…
In honoring the seminal contribution of Henry Eyring and Michael Polanyi who first introduced the concept of potential energy surfaces (PESs) to describe chemical reactions in gas-phase [Z. Phys. Chem. 12, 279-311, (1931)], this work comes…
By simulating the dissociation of O2 molecules on the Be(0001) surface using the first-principles molecular dynamics approach, we propose a new atomistic model for the surface oxidation of sp metals. In our model, only the dissociation of…
A novel quantum dynamical method to simulate vibronic reaction dynamics in molecules at metal surfaces is proposed. The method is based on the hierarchical quantum master equation approach and uses a discrete variable representation of the…
The interaction of hydrogen with many transition metal surfaces is characterized by a coexistence of activated with non-activated paths to adsorption with a broad distribution of barrier heights. By performing six-dimensional quantum…
The coupling of excited states and ionic dynamics is the basic and challenging point for the materials response at extreme conditions. In laboratory, the intense laser produces transient nature and complexity with highly nonequilibrium…
Ab initio molecular dynamics (AIMD) simulations employing density functional theory (DFT) and plane waves are routinely carried out using density functionals at the level of Generalized Gradient Approximation (GGA). AIMD simulations…