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Local Geometry, Structure and Electronic Resonances Enhancing the SFG Signal from CO on Ir Surfaces.

Xia Li1, Stefania Baronio2, Susanne Gross1

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The Journal of Physical Chemistry. C, Nanomaterials and Interfaces
|July 16, 2025
PubMed
Summary

Sum frequency generation (SFG) spectroscopy revealed an eightfold increase in CO adsorption signal intensity on rough iridium surfaces compared to smooth ones. This enhancement is attributed to localized surface plasmon resonances excited by surface roughness.

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Area of Science:

  • Surface Science
  • Spectroscopy
  • Materials Science

Background:

  • Understanding adsorbate behavior on metal surfaces is crucial for catalysis and materials science.
  • Sum frequency generation (SFG) spectroscopy is a powerful vibrational spectroscopy technique for studying surfaces.
  • Iridium (Ir) surfaces are important in various catalytic applications.

Purpose of the Study:

  • To investigate the effect of surface roughness on CO adsorption on Ir(111) using SFG spectroscopy.
  • To elucidate the underlying mechanisms responsible for observed signal intensity differences.
  • To characterize the surface properties influencing adsorbate-surface interactions.

Main Methods:

  • Sum frequency generation (SFG) spectroscopy was the primary technique.
  • Surface characterization included Auger electron spectroscopy (AES), low energy ion scattering (LEIS), low energy electron diffraction (LEED), and scanning tunneling microscopy (STM).
  • Comparative studies were performed on smooth and rough Ir(111) surfaces.

Main Results:

  • A significant (approximately eightfold) increase in resonant SFG signal intensity for the CO C-O stretch mode was observed on rough Ir(111) compared to smooth Ir(111).
  • Surface characterization confirmed the presence of sputter-induced local roughness (grains) on the modified surface.
  • Various factors like coverage, lateral interactions, molecular hyperpolarizability, adsorption geometry, Fermi resonances, adsorbate hot vibrational bands, and surface plasmons were considered.

Conclusions:

  • The enhanced SFG signal on rough Ir(111) is primarily attributed to the excitation of localized surface plasmon resonances (LSPR) facilitated by surface roughness.
  • LSPR enhances light-induced excitation, leading to the observed signal amplification.
  • Surface morphology plays a critical role in modulating spectroscopic signals of adsorbed molecules.