A Linearized Semiclassical dynamics study of the multi-quantum vibrational relaxation of NO scattering from a Au(111) Surface

Abstract

The vibrational relaxation of NO molecules scattering from an Au(111) surface has served as the focus of efforts to understand nonadiabatic energy transfer at metal-molecule interfaces. Experimental measurements and previous theoretical efforts suggest that multi-quantal NO vibrational energy relaxation occurs via electron hole pair excitations in the metal. Here, using a Linearized Semiclassical approach, we accurately predict the vibrational relaxation of NO from ${\nu }_i=3$ state for different incident translational energies. We also accurately capture the central role of transient electron transfer from the metal to the molecule in mediating vibrational relaxation process, but fall short of quantitatively predicting the full extent of multi-quantum relaxation for high incident vibrational excitations (${\nu }_i=16$).

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Cited by in corpus (4)

• Nonadiabatic Field: A Conceptually Novel Approach for Nonadiabatic Quantum Molecular Dynamics
• Nonadiabatic H-Atom Scattering Channels on Ge(111) Elucidated by the Hierarchical Equations of Motion
• Semiclassical Dynamics in Wigner Phase Space I : Adiabatic Hybrid Wigner Dynamics
• Semiclassical Dynamics in Wigner Phase Space II : nonadiabatic Hybrid Wigner Dynamics