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 language | English |
|---|---|
| Pages (from-to) | 849-854 |
| Number of pages | 6 |
| Journal | Journal of the American Chemical Society |
| Volume | 131 |
| Issue number | 2 |
| DOIs | |
| Publication status | Published - Jan 21 2009 |
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ASJC Scopus subject areas
- Chemistry(all)
- Catalysis
- Biochemistry
- Colloid and Surface Chemistry
Cite this
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 journal › Article
}
TY - JOUR
T1 - Surface-enhanced Raman excitation spectroscopy of a single rhodamine 6G molecule
AU - Dieringer, Jon A.
AU - Wustholz, Kristin L.
AU - Masiello, David J.
AU - Camden, Jon P.
AU - Kleinman, Samuel L.
AU - Schatz, George C
AU - Van Duyne, Richard P.
PY - 2009/1/21
Y1 - 2009/1/21
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=67749103812&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=67749103812&partnerID=8YFLogxK
U2 - 10.1021/ja8080154
DO - 10.1021/ja8080154
M3 - Article
C2 - 19140802
AN - SCOPUS:67749103812
VL - 131
SP - 849
EP - 854
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 2
ER -