An improved static corrugation model.

Area of Science:

• Physical Chemistry
• Surface Science
• Computational Chemistry

Background:

• Accurately modeling surface temperature effects on H2 dissociation on metal surfaces like Cu(111) is computationally demanding.
• Current state-of-the-art methods, such as Ab initio Molecular Dynamics (AIMD), provide accuracy but are prohibitively expensive for extensive parameter testing.

Purpose of the Study:

• To develop a computationally efficient and chemically accurate model for describing the dissociation of H2 and D2 on Cu(111).
• To investigate the surface temperature effects on reaction and scattering probabilities.

Main Methods:

• A novel static corrugation model was developed, incorporating effective three-body interactions and H2-bond dependence.
• The model was fitted to density functional theory (DFT) energies derived from 15,113 distinct configurations.
• Reaction and rovibrational (in)elastic scattering probabilities were computed using the developed model.

Main Results:

• The static corrugation model demonstrated good agreement with experimental and AIMD results for H2 and D2 dissociation on Cu(111).
• A consistent deviation from experimental data was observed for the reaction of low-energy H2 (v=0, J=0), predicted by both AIMD and the new model.

Conclusions:

• The developed static corrugation model provides a computationally feasible and accurate approach for studying surface dissociation reactions.
• The model's agreement with experiments highlights its potential for broader applications in surface chemistry, despite a noted discrepancy in specific low-energy reaction channels.