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ReactionBarriometry Report Summary

Project ID: 338580
Funded under: FP7-IDEAS-ERC
Country: Netherlands

Mid-Term Report Summary - REACTIONBARRIOMETRY (Towards a chemically accurate description of reactions on metal surfaces)

This project attacks the 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 computation of chemically accurate barrier heights for reactions with metal surfaces of catalytic interest, using so-called first principles methods. In the first challenge addressed, to establish the accuracy of a new method for computing interaction energies between molecules we will test whether a semi-empirical approach to density functional theory (a popular method for computing interaction energies for molecular systems), the so-called specific reaction parameter density functional theory (SRP-DFT), can describe reactions like dissociation of molecular nitrogen on a ruthenium surface, of methane on a platinum surface, and of molecular hydrogen on platinum containing surfaces of catalytic interest with "chemical accuracy", i.e., to within 1 kcal/mol. This challenge has already been met for the hardest case (methane, albeit for a nickel surface rather than a platinum surface). We will try to put this SRP-DFT approach on an first principles basis by fitting SRP density functionals to calculations with the so-called Quantum Monte-Carlo method, which is a first principles method. An important step in this direction has already been taken: we have evaluated the accuracy of the Quantum Monte Carlo method for molecules containing metal atoms of the type we are interested in (so-called transition metals), and the results look promising. Second, we aim to achieve an accurate description of the effect of motions of the surface atoms on reaction through implementing so-called Ab Initio Molecular Dynamics (AIMD) calculations on several systems. In AIMD, forces acting between the atoms are calculated directly ("on-the-fly") while the simulation proceeds, from first principles. Third, we additionally aim to achieve an accurate description of the effect of electronic excitations in the metal on reaction in systems like molecular nitrogen interacting with a ruthenium surface by implementing a new method called Ab Initio Molecular Dynamics with Electronic Friction. The fourth goal is to achieve an accurate quantum mechanical dynamical description of the reaction of hydrogen atom containing polyatomic molecules at surfaces at incidence energies of catalytic interest (i.e., low energies). The quantum dynamics calculations will treat all molecular degrees of freedom and one surface mode, which will ultimately enable detailed interpretations of exciting experiments.

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