Reactions at surfaces studied by ab initio dynamics calculations

TL;DR

This paper reviews the advancements in ab initio dynamics simulations for surface reactions, highlighting the ability to treat hydrogen dissociation on various surfaces from first principles without adjustable parameters.

Contribution

It introduces the application of fully quantum dynamic simulations to surface reactions, especially hydrogen dissociation, using first-principles methods with recent methodological developments.

Findings

Quantum dynamic treatment of hydrogen dissociation on metal surfaces

Simulation of reactions on semiconductor and passivated surfaces

Progress in laser-induced desorption modeling

Abstract

Due to the development of efficient algorithms and the improvement of computer power it is now possible to map out potential energy surfaces (PES) of reactions at surfaces in great detail. This achievement has been accompanied by an increased effort in the dynamical simulation of processes on surfaces. The paradigm for simple reactions at surfaces -- the dissociation of hydrogen on metal surfaces -- can now be treated fully quantum dynamically in the molecular degrees of freedom from first principles, i.e., without invoking any adjustable parameters. This relatively new field of ab initio dynamics simulations of reactions at surfaces will be reviewed. Mainly the dissociation of hydrogen on clean and adsorbate covered metal surfaces and on semiconductor surfaces will be discussed. In addition, the ab initio molecular dynamics treatment of reactions of hydrogen atoms with hydrogen-passivated semiconductor surfaces and recent achievements in the ab initio description of laser-induced desorption and further developments will be addressed.