Towards a chemically accurate description of reactions on metal surfaces
How can we make make accurate predictions for reactions of molecules on metal surfaces?
The proposed research will attack four major challenges facing theorists who aim to make accurate predictions for reactions of molecules on metal surfaces. The research is curiosity driven, but also of practical importance to an accurate description of heterogeneous catalysis, which enables the production of > 90% of man made chemicals. The central goal is to enable the ab initio computation of chemically accurate barrier heights for reactions with metal surfaces of catalytic interest.
In the first challenge addressed, to establish the accuracy of a new electronic structure method we will test whether specific reaction parameter density functional theory (SRP-DFT) can describe reactions of catalytic interest, like dissociation of N 2, CH 4, and H 2 on metal surfaces, with chemical accuracy. The researchers will try to put SRP-DFT, which was first used semi-empirically, on an ab initio basis. Second, they aim to achieve an accurate description of the effect of surface phonons on reaction through implementing Ab Initio Molecular Dynamics calculations on systems like methane interacting with Pt surfaces, and N 2 reacting on metal surfaces. Third, the researchers additionally aim to achieve an accurate description of the effect of electron-hole pair excitation on reaction in specific systems by implementing a new method called Ab Initio Molecular Dynamics with Electronic Friction. The fourth goal is to achieve an accurate quantum dynamical description of the reaction of hydrogen containing polyatomic molecules at surfaces at incidence energies of catalytic interest (in the quantum regime). The quantum dynamics calculations will treat all molecular degrees of freedom and one surface mode, which will ultimately enable detailed interpretations of recently observed mode-selectivity, bond-selectivity, and steric effects in the reaction of methane with metal surfaces.