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arXiv · 1506.06877

Electronic friction-based vibrational lifetimes of molecular adsorbates: Beyond the independent atom approximation

Simon P. Rittmeyer·Jörg Meyer·J. Iñaki Juaristi·Karsten Reuter
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Abstract

We assess the accuracy of vibrational damping rates of diatomic adsorbates on metal surfaces as calculated within the local-density friction approximation (LDFA). An atoms-in-molecules (AIM) type charge partitioning scheme accounts for intra-molecular contributions and overcomes the systematic underestimation of the non-adiabatic losses obtained within the prevalent independent atom approximation. The quantitative agreement obtained with theoretical and experimental benchmark data suggests the LDFA-AIM as an efficient and reliable approach to account for electronic dissipation in ab initio molecular dynamics simulations of surface chemical reactions.

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Simon P. Rittmeyer, Jörg Meyer, J. Iñaki Juaristi, Karsten Reuter. 2015-06-23. Electronic friction-based vibrational lifetimes of molecular adsorbates: Beyond the independent atom approximation. https://doi.org/10.1103/physrevlett.115.046102

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