Ab initio simulation of the spin transition during chemisorption: H/Al(111)

Area of Science:

• Surface science
• Quantum chemistry
• Computational physics

Background:

• Chemisorption involves chemical bonding between atoms/molecules and a surface.
• Understanding electron dynamics is crucial for surface reactions.
• Al(111) is a model system for studying metal surface interactions.

Purpose of the Study:

• To simulate and analyze electronically nonadiabatic effects during hydrogen chemisorption on Al(111).
• To investigate energy dissipation and electron-hole pair excitations.
• To validate theoretical models for surface processes.

Main Methods:

• Ab initio simulations using time-dependent density-functional theory (TDDFT) for electrons.
• Ehrenfest dynamics employed for nuclear motion.
• Calculation of dissipated energy and electron-hole pair excitation spectra.

Main Results:

• Strongly nonadiabatic effects were identified near the spin transition of hydrogen atoms.
• Dissipated energy and electron-hole pair excitation spectra were calculated.
• The study confirmed the validity of the Newns-Anderson-model approach by Mizielinski et al.

Conclusions:

• Simulations provide insights into the physical processes governing internal exoelectron emission.
• Electronically nonadiabatic effects play a significant role in hydrogen-Al(111) chemisorption.
• The findings contribute to a deeper understanding of surface reaction dynamics and electron emission phenomena.