Nonadiabatic Vibrational Damping of Molecular Adsorbates: Insights into 
Electronic Friction and the Role of Electronic Coherence

Rittmeyer, Simon P.; Meyer, Jörg; Reuter, Karsten

doi:10.1103/PhysRevLett.119.176808

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Nonadiabatic Vibrational Damping of Molecular Adsorbates: Insights into Electronic Friction and the Role of Electronic Coherence

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Rittmeyer, S. P., Meyer, J., & Reuter, K. (2017). Nonadiabatic Vibrational Damping of Molecular Adsorbates: Insights into Electronic Friction and the Role of Electronic Coherence. Physical Review Letters, 119(17): 176808. doi:10.1103/PhysRevLett.119.176808.

Cite as: https://hdl.handle.net/21.11116/0000-000A-AC43-9

Abstract

We present a perturbation approach rooted in time-dependent density-functional theory to calculate electron-hole (e−h) pair excitation spectra during the nonadiabatic vibrational damping of adsorbates on metal surfaces. Our analysis for the benchmark systems CO on Cu(100) and Pt(111) elucidates the surprisingly strong influence of rather short electronic coherence times. We demonstrate how in the limit of short electronic coherence times, as implicitly assumed in prevalent quantum nuclear theories for the vibrational lifetimes as well as electronic friction, band structure effects are washed out. Our results suggest that more accurate lifetime or chemicurrentlike experimental measurements could characterize the electronic coherence.