Abstract
The reaction between an impinging H atom and a Cl atom adsorbed on Au(111), which is a prototype for the Eley-Rideal mechanism, is investigated using ab initio molecular dynamics at different incidence angles. The reaction yielding gaseous HCl with large internal excitation proceeds via both direct and hot-atom mechanisms. Significant energy exchange with both surface phonons and electron-hole pairs has been observed. However, their impact on the reactivity and final state distributions was found to be limited, thanks to the large exothermicity and small barrier of the reaction.
Highlights
Fundamental molecule-surface encounters are the basis for understanding many interfacial problems such as aerosol chemistry, corrosion, materials processing, heterogeneous catalysis, and plasma chemistry
The reaction between an impinging H atom and a Cl atom adsorbed on Au(111), which is a prototype for the Eley-Rideal mechanism, is investigated using ab initio molecular dynamics at different incidence angles
We present in this work extensive ab initio molecular dynamics (AIMD) simulations of a prototypical Eley-Rideal type reaction between impinging H atoms and chlorine atoms adsorbed on Au(111)
Summary
Fundamental molecule-surface encounters are the basis for understanding many interfacial problems such as aerosol chemistry, corrosion, materials processing, heterogeneous catalysis, and plasma chemistry. A less-investigated aspect in ER/HA dynamics is the involvement of the substrate surface and the extent of energy exchange. For example, demonstrated that impinging H atoms can quickly dissipate their energy through coupling to low-energy EHPs in the metal surface.. It is imperative to include both dissipation channels in dynamical studies, if they involve light atoms or adsorbates.. We investigate the dynamics of a prototypical ER reaction, in which a gas phase H atom reacts with a Cl atom adsorbed on the Au(111) surface to form desorbed HCl, using ab initio molecular dynamics (AIMD).. In addition to the AIMD studies, we have carried out AIMD with electronic friction (AIMDEF) calculations in which the possible involvement of EHPs in the energy dissipation of hot H atoms is explored with the LDFA approach.. The AIMD approach has very recently been used successfully in studying HCl scattering and dissociation on Au(111). In addition to the AIMD studies, we have carried out AIMD with electronic friction (AIMDEF) calculations in which the possible involvement of EHPs in the energy dissipation of hot H atoms is explored with the LDFA approach. The AIMDEF approach eliminates the uncertainties in the previous empirical treatment of the EHP effects. the results presented here are expected to provide a much more quantitative and complete picture of the ER/HA dynamics of the title reaction and the role of energy dissipation
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