Efficient implementation and performance analysis of the independent electron surface hopping method for dynamics at...

Area of Science:

• Computational chemistry
• Surface science
• Quantum dynamics

Background:

• Simulating molecular dynamics at metal surfaces requires accounting for nonadiabatic effects.
• Electron-hole pair excitations significantly influence molecular behavior on surfaces.

Purpose of the Study:

• To present a transparent, reliable, and efficient implementation of Independent Electron Surface Hopping (IESH).
• To demonstrate IESH's capability in predicting scattering and desorption probabilities.
• To explore modifications of IESH for external bias potentials.

Main Methods:

• Implementation of the Independent Electron Surface Hopping (IESH) algorithm.
• Application to model Hamiltonians and full-dimensional atomistic systems.
• Comparison with hierarchical quantum master equation for biased systems.

Main Results:

• IESH accurately predicts scattering and desorption probabilities for various systems.
• The modified IESH algorithm shows good agreement with quantum master equation results under bias.
• IESH proves effective for simulating coupled electron-nuclear dynamics.

Conclusions:

• IESH is a practical and efficient computational tool for studying electron-nuclear dynamics at metal surfaces.
• The method is particularly useful for simulating highly energetic scattering events.
• IESH provides a reliable approach for understanding surface chemistry and physics.