Analysis of Energy Dissipation Channels in a Benchmark System of Activated Dissociation: N-2 on Ru(0001)

K Shakouri and J Behler and J Meyer and GJ Kroes, JOURNAL OF PHYSICAL CHEMISTRY C, 122, 23470-23480 (2018).

DOI: 10.1021/acs.jpcc.8b06729

The excitation of electron-hole pairs in reactive scattering of molecules at metal surfaces often affects the physical and dynamical observables of interest, including the reaction probability. Here, we study the influence of electron-hole pair excitation on the dissociative chemisorption of N-2 on Ru(0001) using the local density friction approximation method. The effect of surface atom motion has also been taken into account by a high-dimensional neural network potential. Our nonadiabatic molecular dynamics simulations with electronic friction show that the reaction of N-2 is more strongly affected by the energy transfer to surface phonons than by the energy loss to electron-hole pairs. The discrepancy between the computed reaction probabilities and experimental results is within the experimental error both with and without friction; however, the incorporation of electron-hole pairs yields somewhat better agreement with experiments, especially at high collision energies. We also calculate the vibrational efficacy for the N-2 + Ru(0001) reaction and demonstrate that the N-2 reaction is more enhanced by exciting the molecular vibrations than by adding an equivalent amount of energy into translation.

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