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Nonadiabatic effects in the dissociation of oxygen molecules at the Al(111) surface

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Behler,  Jörg
Theory, Fritz Haber Institute, Max Planck Society;

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Reuter,  Karsten
Theory, Fritz Haber Institute, Max Planck Society;

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Scheffler,  Matthias
Theory, Fritz Haber Institute, Max Planck Society;

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PRB-77-115421-2008.pdf
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Citation

Behler, J., Reuter, K., & Scheffler, M. (2008). Nonadiabatic effects in the dissociation of oxygen molecules at the Al(111) surface. Physical Review B, 77(11), 115421-1-115421-16. Retrieved from http://dx.doi.org/10.1103/PhysRevB.77.115421.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0010-FD43-4
Abstract
The measured low initial sticking probability of oxygen molecules at the Al(111) surface that had puzzled the field for many years was recently explained in a nonadiabatic picture invoking spin-selection rules [J. Behler et al., Phys. Rev. Lett. 94, 036104 (2005)]. These selection rules tend to conserve the initial spin-triplet character of the free O2 molecule during the molecule’s approach to the surface. A locally constrained density-functional theory approach gave access to the corresponding potential-energy surface (PES) seen by such an impinging spin-triplet molecule and indicated barriers to dissociation which reduce the sticking probability. Here, we further substantiate this nonadiabatic picture by providing a detailed account of the employed approach. Building on the previous work, we focus, in particular, on inaccuracies in present-day exchange-correlation functionals. Our analysis shows that small quantitative differences in the spin-triplet constrained PES obtained with different gradient-corrected functionals have a noticeable effect on the lowest kinetic energy part of the resulting sticking curve.