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arXiv · 1705.09753

Mode specific electronic friction in dissociative chemisorption on metal surfaces: H$_2$ on Ag(111)

Reinhard J. Maurer·Bin Jiang·Hua Guo·John C. Tully
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Abstract

Electronic friction and the ensuing nonadiabatic energy loss play an important role in chemical reaction dynamics at metal surfaces. Using molecular dynamics with electronic friction evaluated on-the-fly from Density Functional Theory, we find strong mode dependence and a dominance of nonadiabatic energy loss along the bond stretch coordinate for scattering and dissociative chemisorption of H$_2$ on the Ag(111) surface. Exemplary trajectories with varying initial conditions indicate that this mode-specificity translates into modulated energy loss during a dissociative chemisorption event. Despite minor nonadiabatic energy loss of about 5\%, the directionality of friction forces induces dynamical steering that affects individual reaction outcomes, specifically for low-incidence energies and vibrationally excited molecules. Mode-specific friction induces enhanced loss of rovibrational rather than translational energy and will be most visible in its effect on final energy distributions in molecular scattering experiments.

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Reinhard J. Maurer, Bin Jiang, Hua Guo, John C. Tully. 2017-05-27. Mode specific electronic friction in dissociative chemisorption on metal surfaces: H$_2$ on Ag(111). https://doi.org/10.1103/physrevlett.118.256001

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