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Modeling Surface-Enhanced Spectroscopy With Perturbation Theory.

Niclas S Mueller1, Stephanie Reich1

  • 1Department of Physics, Freie Universität Berlin, Berlin, Germany.

Frontiers in Chemistry
|August 6, 2019
PubMed
Summary

This study models surface-enhanced Raman scattering (SERS) using perturbation theory, revealing plasmon excitation as key to Raman enhancement. The findings aid in designing better SERS substrates and interpreting experimental results.

Keywords:
optical interferenceperturbation theoryplasmonicssecond quantization formalismsurface-enhanced Raman spectroscopy (SERS)

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Area of Science:

  • Plasmonics
  • Spectroscopy
  • Theoretical Chemistry

Background:

  • Surface-enhanced Raman scattering (SERS) relies on plasmonic enhancement for increased sensitivity.
  • Understanding the theoretical underpinnings of SERS is crucial for substrate design and application.
  • Existing models often require experimental validation for predictive accuracy.

Purpose of the Study:

  • To develop a theoretical model for the plasmonic enhancement mechanism in SERS using perturbation theory.
  • To explain the role of plasmon excitation at incident and scattered light wavelengths in SERS.
  • To provide a framework for predictive design of SERS substrates and interpretation of experimental data.

Main Methods:

  • Employing perturbation theory to model the plasmonic enhancement in SERS.
  • Treating plasmon excitation as an integral part of the Raman scattering process.
  • Calculating optical absorption cross sections of plasmonic nanoparticles using the developed theory.

Main Results:

  • Derived an analytic expression for the Raman cross section, explaining resonance Raman measurements.
  • Identified additional resonances corresponding to plasmon excitation at incident and Raman-scattered light wavelengths.
  • Determined that renormalization of coupling matrix elements is necessary for accurate optical absorption cross-section calculations.
  • Demonstrated interference of scattering channels as critical for understanding SERS enhancement below 10^3.

Conclusions:

  • The perturbation theory model accurately describes SERS enhancement mechanisms.
  • The model provides insights into the excitation energy dependence of SERS.
  • This theoretical framework facilitates the rational design of advanced SERS substrates.