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Imaging Electric Fields in SERS and TERS Using the Vibrational Stark Effect.

James M Marr1, Zachary D Schultz

  • 1University of Notre Dame, Department of Chemistry and Biochemistry, Notre Dame, IN 46556.

The Journal of Physical Chemistry Letters
|November 26, 2013
PubMed
Summary

Researchers directly measured electric fields in surface-enhanced Raman scattering (SERS) and tip-enhanced Raman scattering (TERS) experiments. Using the vibrational Stark effect on cyanide molecules on gold surfaces, they quantified localized electric fields, correlating them with Raman signal enhancements.

Keywords:
RamanSERSTERSnitrileplasmonicsvibrational stark effect

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Area of Science:

  • Surface Science
  • Spectroscopy
  • Nanotechnology

Background:

  • Electric fields in Raman enhancement are usually inferred indirectly from scattering intensity.
  • Direct measurement of electric fields in Surface-Enhanced Raman Scattering (SERS) and Tip-Enhanced Raman Scattering (TERS) is crucial for understanding enhancement mechanisms.
  • The vibrational Stark effect offers a potential method for probing local electric fields.

Purpose of the Study:

  • To directly measure electric fields present during SERS and TERS experiments.
  • To utilize the vibrational Stark effect of a nitrile reporter group (cyanide) on a gold surface for electric field quantification.
  • To correlate measured electric fields with Raman enhancement factors and surface topography.

Main Methods:

  • Employed the vibrational Stark effect using cyanide (CN) as a reporter molecule on electroplated gold (Au) surfaces.
  • Investigated SERS activity on Au surfaces, analyzing Stark shifts in relation to surface roughness and co-adsorbed molecules (thiophenol).
  • Utilized gap-mode Tip-Enhanced Raman Scattering (TERS) with a gold nanoparticle tip to probe electric fields in the nanogap.

Main Results:

  • Larger Stark shifts were observed on electroplated Au surfaces with higher SERS activity, particularly near edges and rough areas.
  • The magnitude of the Stark shift correlated with the intensity of co-adsorbed thiophenol, indicating field sensitivity.
  • TERS experiments revealed dramatic shifts in the CN stretch frequency, correlating with enhancement factors up to 10^13, and indicated highly localized fields.

Conclusions:

  • Changes in nitrile stretch frequency provide a direct and quantitative measurement of electric fields in SERS and TERS.
  • The study demonstrates the utility of the vibrational Stark effect for mapping and quantifying localized electric fields in plasmonic nanostructures.
  • Electric field localization is a key factor in achieving ultra-high Raman enhancement, as observed in gap-mode TERS.