The relevance of structural variability in the time-domain for computational reflection anisotropy spectroscopy at...

Area of Science:

• Surface science
• Computational electrochemistry
• Spectroscopy

Background:

• Solid-liquid interface structure dictates electrochemical reactions.
• Traditional surface science methods are limited in liquid electrolytes.
• In operando investigation of these interfaces is crucial but challenging.

Purpose of the Study:

• To investigate the temporal evolution of the Au(110) missing row reconstruction in water.
• To combine ab initio molecular dynamics with computational spectroscopy for interface analysis.
• To provide atomistic insights into the dynamic solid-liquid interface.

Main Methods:

• Ab initio molecular dynamics simulations.
• Computational spectroscopy.
• Reflection anisotropy spectroscopy (RAS) data analysis.

Main Results:

• Observed significant changes in the time evolution of RA spectra.
• Provided explanations for intensity differences between theory and experiment.
• Highlighted the importance of structural surface/interface variability.

Conclusions:

• The dynamic nature of solid-liquid interfaces significantly impacts spectroscopic responses.
• Reflection anisotropy spectroscopy (RAS) is a powerful tool for probing dynamic electrochemical interfaces.
• Accounting for interface dynamics is essential for accurate theoretical interpretation of experimental RAS data.