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Classical Model of Surface Enhanced Infrared Absorption (SEIRA) Spectroscopy.

Yuan Gao1, D E Aspnes2, Stefan Franzen1

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The Journal of Physical Chemistry. A
|January 10, 2022
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This study explores molecule-plasmon interactions using a novel semiconductor film for enhanced infrared absorption (SEIRA) and Raman scattering (SERS). The developed model accurately predicts SEIRA signals and enhancement factors, validating the approach for advanced spectroscopy.

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Area of Science:

  • Plasmonics
  • Spectroscopy
  • Materials Science

Background:

  • Molecule-plasmon interactions underpin surface-enhanced infrared absorption (SEIRA) and surface-enhanced Raman scattering (SERS).
  • Classical electromagnetic theory provides a framework for understanding these interactions when molecular transition moments are properly described.
  • Previous work established a classical model for Raman excitation profiles.

Purpose of the Study:

  • To generalize the understanding of plasmon-molecule interactions by investigating the SEIRA signal of N2O on a Dy-doped CdO (CdO:Dy) film.
  • To explore the use of semiconductor materials with tunable plasmon dispersion for enhanced vibrational spectroscopy.
  • To validate a classical model predicting SEIRA phase behavior and enhancement factors.

Main Methods:

  • Utilized a Dy-doped CdO (CdO:Dy) film with tunable near- and mid-infrared plasmon dispersion.
  • Employed the Kretschmann configuration with CaF2 prism and MgO substrate for SEIRA measurements.
  • Developed and applied a classical model to predict SEIRA signals and enhancement factors.

Main Results:

  • The CdO:Dy film demonstrated tunable plasmon dispersion interacting with vibrational transitions.
  • The classical model successfully predicted the phase behavior of SEIRA.
  • A calculated SEIRA enhancement factor of 6.2 was achieved, closely matching the experimental value of 6.8 ± 0.5 relative to an Au control.

Conclusions:

  • Dy-doped CdO is a promising material for SEIRA and SERS applications due to its tunable plasmonics.
  • The classical electromagnetic model effectively describes molecule-plasmon interactions in SEIRA.
  • This work advances the understanding and application of plasmon-enhanced vibrational spectroscopies.