Surface-enhanced Raman excitation spectroscopy of a single rhodamine 6G molecule

Jon A. Dieringer, Kristin L. Wustholz, David J. Masiello, Jon P. Camden, Samuel L. Kleinman, George C Schatz, Richard P. Van Duyne

Research output: Contribution to journalArticle

239 Citations (Scopus)

Abstract

The surface-enhanced Raman excitation profiles (REPs) of rhodamine 6G (R6G) on Ag surfaces are studied using a tunable optical parametric oscillator excitation source and versatile detection scheme. These experiments afford the ability to finely tune the excitation wavelength near the molecular resonance of R6G (i.e., ~500-575 nm) and perform wavelength-scanned surface-enhanced Raman excitation measurements of a single molecule. The ensemble-averaged surface-enhanced REPs are measured for collections of molecules on Ag island films. The relative contributions of the 0-0 and 0-1 vibronic transitions to the surface-enhanced REPs vary with vibrational frequency. These results highlight the role of excitation energy in determining the resonance Raman intensities for R6G on surface-enhancing nanostructures. Single-molecule measurements are obtained from individual molecules of R6G on Ag colloidal aggregates, where single-molecule junctions are located using the isotope-edited approach. Overall, single-molecule surface-enhanced REPs are narrow in comparison to the ensemble-averaged excitation profiles due to a reduction in inhomogeneous broadening. This work describes the first Raman excitation spectroscopy studies of a single molecule, revealing new information previously obscured by the ensemble.

Original languageEnglish
Pages (from-to)849-854
Number of pages6
JournalJournal of the American Chemical Society
Volume131
Issue number2
DOIs
Publication statusPublished - Jan 21 2009

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Raman Spectrum Analysis
Spectroscopy
Molecules
Nanostructures
Islands
Isotopes
Optical parametric oscillators
Wavelength
Excitation energy
Vibrational spectra
rhodamine 6G

ASJC Scopus subject areas

  • Chemistry(all)
  • Catalysis
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Dieringer, J. A., Wustholz, K. L., Masiello, D. J., Camden, J. P., Kleinman, S. L., Schatz, G. C., & Van Duyne, R. P. (2009). Surface-enhanced Raman excitation spectroscopy of a single rhodamine 6G molecule. Journal of the American Chemical Society, 131(2), 849-854. https://doi.org/10.1021/ja8080154

Surface-enhanced Raman excitation spectroscopy of a single rhodamine 6G molecule. / Dieringer, Jon A.; Wustholz, Kristin L.; Masiello, David J.; Camden, Jon P.; Kleinman, Samuel L.; Schatz, George C; Van Duyne, Richard P.

In: Journal of the American Chemical Society, Vol. 131, No. 2, 21.01.2009, p. 849-854.

Research output: Contribution to journalArticle

Dieringer, JA, Wustholz, KL, Masiello, DJ, Camden, JP, Kleinman, SL, Schatz, GC & Van Duyne, RP 2009, 'Surface-enhanced Raman excitation spectroscopy of a single rhodamine 6G molecule', Journal of the American Chemical Society, vol. 131, no. 2, pp. 849-854. https://doi.org/10.1021/ja8080154
Dieringer, Jon A. ; Wustholz, Kristin L. ; Masiello, David J. ; Camden, Jon P. ; Kleinman, Samuel L. ; Schatz, George C ; Van Duyne, Richard P. / Surface-enhanced Raman excitation spectroscopy of a single rhodamine 6G molecule. In: Journal of the American Chemical Society. 2009 ; Vol. 131, No. 2. pp. 849-854.
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