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F. Libisch:
"Quantum-Mechanical Embedding Methods for Surface Catalysis";
Vortrag: MRS Fall Meeting 2019, Boston (eingeladen); 01.12.2019 - 06.12.2019.

The charge transfer reactions upon dissociative absorption of O2 on metal surfaces is critical for many catalytic processes, yet poses a challenging problem for state-of-the-art ab-initio theoretical modeling. For example, the experimentally observed activation barrier for O2 dissociation on Al (111) is not captured by conventional density functional theory. However, accurate wavefunction-based methods that are well suited to handle the multireference character of the charge transfer state are ill suited to describe extended metal surfaces. Embedding methods offer a way forward, by combining highly accurate wave-function based approaches at the absorption site with an environment described by density functional theory. In the case of O2 on Al(111), such an approach naturally yields an adiabatic barrier [1]. I review our recent advances and challenges in solving catalytic problems using embedding methods, including the build-up of six-dimensional potential energy surface (PES) suited for quasi-classical trajectory calculations [2], projection-based approaches that enable freeze-thaw cycles, and the extension to high-level methods such as Quantum Monte Carlo or Coupled Cluster that can treat periodic boundary conditions.

[1] F. Libisch, C. Huang, and E. A. Carter Accounts of Chemical Research, 47, 2768 (2014)
[2] R. Yin, Y. Zhang, F. Libisch, E. A. Carter, H. Guo, and B. Jiang J. Chem. Phys. Lett. 9, 3271 (2018)

Catalysis, Embedding