Surface diffusion of carbon monoxide on Ru(001) studied using laser-induced thermal desorption

Deckert, A. A.; Brand, J. L.; Arena, M. V.; George, Steven M.

doi:10.1016/0039-6028(89)90012-5

Cited by 83 publications

(38 citation statements)

References 56 publications

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“…For MDEF-GLO these values are further enhanced by about 30%. The FL-derived diffusion coefficients are up to five orders of magnitude larger than purely thermal diffusion coefficients for CO/Ru(0001), measured at 300 K [36]. For example, at a coverage of 0.27 (comparable to ours), D ∼ 3 × 10 −9 cm 2 /s was reported in Ref.…”

Section: B Laser Induced Hot-electron Mediated Surface Diffusionmentioning

confidence: 75%

“…For example, at a coverage of 0.27 (comparable to ours), D ∼ 3 × 10 −9 cm 2 /s was reported in Ref. [36].…”

Section: B Laser Induced Hot-electron Mediated Surface Diffusionmentioning

confidence: 83%

“…Diffusion, on the other hand, of the entire molecule is possible at much lower energies, with minimum barriers for top-to-top diffusion of around 240 meV. In the experimental reference [36], activation energies between 480 and 270 meV were reported for diffusion, depending on coverage. We shall return to this issue below.…”

Section: B Substrate Phonons: Mdef-glo Modelmentioning

confidence: 99%

“…It must be said, however, that according to Ref. [36], E d is strongly coverage dependent, giving E d = 480 meV at a coverage of 0.27. According to Ref.…”

Section: B Laser Induced Hot-electron Mediated Surface Diffusionmentioning

confidence: 99%

“…From an Arrhenius analysis of diffusion, in Ref. [36] an activation energy of 270 meV has been given for a coverage of 0.56, and a prefactor of D 0 = 0.06 cm 2 /s. This activation energy fits nicely to our theoretical values.…”

Section: B Laser Induced Hot-electron Mediated Surface Diffusionmentioning

confidence: 99%

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Femtosecond-laser induced dynamics of CO on Ru(0001): Deep insights from a hot-electron friction model including surface motion

et al. 2016

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A Langevin model accounting for all six molecular degrees of freedom is applied to femtosecond-laser induced, hot-electron driven dynamics of Ru(0001)(2 × 2):CO. In our molecular dynamics with electronic friction approach, a recently developed potential energy surface based on gradient-corrected density functional theory accounting for van der Waals interactions is adopted. Electronic friction due to the coupling of molecular degrees of freedom to electron-hole pairs in the metal are included via a local density friction approximation, and surface phonons by a generalized Langevin oscillator model. The action of ultrashort laser pulses enters through a substrate-mediated, hot-electron mechanism via a time-dependent electronic temperature (derived from a two-temperature model), causing random forces acting on the molecule. The model is applied to laser induced lateral diffusion of CO on the surface, "hot adsorbate" formation, and laser induced desorption. Reaction probabilities are strongly enhanced compared to purely thermal processes, both for diffusion and desorption. Reaction yields depend in a characteristic (nonlinear) fashion on the applied laser fluence, as well as branching ratios for various reaction channels. Computed two-pulse correlation traces for desorption and other indicators suggest that aside from electron-hole pairs, phonons play a non-negligible role for laser induced dynamics in this system, acting on a surprisingly short time scale. Our simulations on precomputed potentials allow for good statistics and the treatment of long-time dynamics (300 ps), giving insight into this system which hitherto has not been reached. We find generally good agreement with experimental data where available and make predictions in addition. A recently proposed laser induced population of physisorbed precursor states could not be observed with the present low-coverage model.

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Section: B Laser Induced Hot-electron Mediated Surface Diffusionmentioning

confidence: 75%

“…For example, at a coverage of 0.27 (comparable to ours), D ∼ 3 × 10 −9 cm 2 /s was reported in Ref. [36].…”

Section: B Laser Induced Hot-electron Mediated Surface Diffusionmentioning

confidence: 83%

Section: B Substrate Phonons: Mdef-glo Modelmentioning

confidence: 99%

“…It must be said, however, that according to Ref. [36], E d is strongly coverage dependent, giving E d = 480 meV at a coverage of 0.27. According to Ref.…”

Section: B Laser Induced Hot-electron Mediated Surface Diffusionmentioning

confidence: 99%

Section: B Laser Induced Hot-electron Mediated Surface Diffusionmentioning

confidence: 99%

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