2013
DOI: 10.1063/1.4811150
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A unifying model for non-adiabatic coupling at metallic surfaces beyond the local harmonic approximation: From vibrational relaxation to scanning tunneling microscopy

Abstract: A model for treating excitation and relaxation of adsorbates at metallic surfaces induced by non-adiabatic coupling is developed. The derivation is based on the concept of resonant electron transfer, where the adsorbate serves as a molecular bridge for the inelastic transition between an electron source and a sink. In this picture, energy relaxation and scanning tunneling microscopy (STM) at metallic surfaces are treated on an equal footing as a quasi-thermal process. The model goes beyond the local harmonic a… Show more

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Cited by 17 publications
(26 citation statements)
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“…Relevant life times from ref. [10] differ only little from the adopted value and if these are used instead of the generic one for the few states for which they are known, results change insignificantly. However, if the values for intrinsic life times change by a factor of 2 or more, so does the calculated diffusion rate [5].…”
Section: Primary Results From These Experiments Is the Intermediate Scmentioning
confidence: 89%
See 1 more Smart Citation
“…Relevant life times from ref. [10] differ only little from the adopted value and if these are used instead of the generic one for the few states for which they are known, results change insignificantly. However, if the values for intrinsic life times change by a factor of 2 or more, so does the calculated diffusion rate [5].…”
Section: Primary Results From These Experiments Is the Intermediate Scmentioning
confidence: 89%
“…Depopulation of vibrational eigenstates of adsorbates on metal substrates via formation of electron-hole pairs is expected to proceed on the picosecond time scale [7,8], or even faster [9,10]. This is about the time scale that can be reached with the 3 He spin-echo technique.…”
Section: Primary Results From These Experiments Is the Intermediate Scmentioning
confidence: 99%
“…As in previous work, 21 the population evolution of the system states driven by the STM is studied using the Pauli master equation…”
Section: Equations Of Motionmentioning
confidence: 99%
“…[18][19][20] A perturbative model for computing rates associated with non-adiabatic coupling of an impurity embedded in a metallic environment was recently introduced. 21 The model includes both energy relaxation/excitation rates due to electronhole pair creation/annihilation in the metallic environment, as well as the STM excitation mechanism. It is based on the evaluation of the vibronic coupling induced by the nuclear kinetic energy operator in the basis of one-electron Kohn-Sham states.…”
Section: Introductionmentioning
confidence: 99%
“…By doing so, well-established expressions for the anharmonic vibrational relaxation rates can be obtained. 42,[44][45][46][47] It is important to note that the effects of IVR, i.e., of intermode coupling induced by the molecular potential, are here explicitly included in the definition of both the relaxation operators and the associate rates.…”
Section: Introductionmentioning
confidence: 99%