Dresden 2014 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 15: Focussed Session: Frontiers of Electronic Structure Theory - Non-equilibrium Phenomena at the Nano-scale II

O 15.7: Vortrag

Montag, 31. März 2014, 17:45–18:00, TRE Ma

Surface chemistry on nanostructured oxides: do we have to go beyond hybrid DFT? — •Daniel Berger, Harald Oberhofer, and Karsten Reuter — Technische Universität München, Germany

Nanostructured oxide surfaces are promising candidates for a wide range of energy and catalysis applications. For first-principles modeling of corresponding surface chemical reactions the current state-of-the-art is generally defined by hybrid-level density-functional theory (DFT). Systematic work assessing the achieved accuracy at this level is nevertheless scarce, also owing to the fact that higher-level reference methods are often not available for standard periodic boundary condition supercell calculations. To this end, we present a study benchmarking semi-local and hybrid DFT against (renormalized) second-order perturbation theory (MP2,rPT2) as recently implemented in the FHI-aims package [1]. We make the efficient usage of the latter theories for oxide surfaces possible through a solid-state embedding framework, in which a central cluster region is described quantum mechanically, the long-range electrostatic interactions in the oxide are accounted for through a polarizable monopole field, and a shell of norm-conserving pseudopotentials correctly connects the two regions. We illustrate the performance of the various levels of theories using the water-splitting reaction at ideal and defected TiO₂(110) surfaces as showcase. [1] X. Ren et al., Phys. Rev. B 88, 035120 (2013)