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F. Libisch:
"Dissociative Chemisorption of O2 on Al(111)";
Vortrag: Workshop: Modern Approaches to Coupling Scales In Materials Simulations, Lenggries, Germany, EU; 02.07.2018 - 04.07.2018.

Dissociative chemisorption of O2 on the Al(111) surface represents a frequently studied prototype for understanding the interaction between O2 and metal surfaces. It is well known that the experimentally observed activation barrier for O2 dissociation is not captured by conventional density functional theory. By contrast, recent embedded correlated wavefunction (ECW) calculations naturally yield an adiabatic barrier [1,2]. However, these ECW calculations have been limited to a static analysis of the reaction pathways and not yet tested by dynamics simulations. We present a global six-dimensional potential energy surface (PES) for this system parameterized with about seven hundred ECW data points. This new PES provides a reasonable description of the global topography of the energy landscape, including site-specific and orientation-dependent activation barriers. Quasi-classical trajectory calculations on this PES semi-quantitatively reproduce both the observed translational energy dependence of the sticking probability and steric effects based on the orientation of the O2 molecules.

[1] F. Libisch, C. Huang, P. Liao, M. Pavone, and E. A. Carter, Physical Review Letters 109, 198303 (2012)
[2] J. Cheng, F. Libisch, and E. A. Carter, J. Phys. Chem. Lett. 6, 1661 (2015)