Development of highly accurate density functionals for H2 dissociation on transition metals

Smeets, E.W.F.

Smeets, E.W.F. (2021)

Development of highly accurate density functionals for H2 dissociation on transition metals

Doctoral Thesis

Metals surfaces form a group of effective catalysts for the reaction of small molecules such as hydrogen (H2). In order to improve the predictive power of theory with respect to the catalytic activity of small molecules reacting at metal surfaces, the way in which metal surfaces modify the potential energy of molecules needs to be understood at a fundamental level. Currently density functional theory (DFT) is the only electronic structure method that is accurate enough to achieve chemical accuracy while being cheap enough to make large comparative studies feasible. The work in this thesis is concerned with the creation of highly accurate density functionals that can give a simultaneously good description of the metal surface, the molecule, and the molecule interacting with the metal surface, as well as the description and simulation of supersonic molecular beam experiments and associative desorption experiments needed to validate the obtained results.

Density functional theory

Specific reaction parameter density functionals

Non-local correlation

Generalized gradient approximation

Meta generalized gradient approximation

Quantum dynamics

Quasi-classical trajectory method

Molecular beam

Associative desorption

Transition metal surfaces