Experimental observation of surface-enhanced coherent anti-Stokes Raman scattering

Liang, Erjun; Weippert, A.; Funk, J.-M.; Materny, A.; Kiefer, W.

doi:10.1016/0009-2614(94)00779-9

Cited by 77 publications

(54 citation statements)

References 18 publications

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“…No enhancement of the CARS spectra was observed for the other wavelengths used. Also, no enhancement effect was observed in the 90° detection scheme in contrast to the earlier observations made when using nanosecond laser pulses [44]. The observed enhancement of CARS spectra from pyridine is seen to have a sensitive dependence on a variety of para meters.…”

Section: Figure 10contrasting

confidence: 59%

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Nonlinear spectroscopy in the near-field: time resolved spectroscopy and subwavelength resolution non-invasive imaging

et al. 2014

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Abstract:The combination of near-field microscopy along with nonlinear optical spectroscopic techniques is presented here. The scanning near-field imaging technique can be integrated with nonlinear spectroscopic techniques to improve spatial and axial resolution of the images. Additionally, ultrafast dynamics can be probed down to nano-scale dimension. The review shows some examples for this combination, which resulted in an exciton map and vibrational contrast images with subwavelength resolution. Results of two-color femtosecond time-resolved pump-probe experiments using scanning near-field optical microscopy (SNOM) on thin films of the organic semiconductor 3,4,9,10 Perylenetetracarboxylic dianhydride (PTCDA) are presented. While nonlinear Raman techniques have been used to obtain highly resolved images in combination with near-field microscopy, the use of femtosecond laser pulses in electronic resonance still constitutes a big challenge. Here, we present our first results on coherent anti-Stokes Raman scattering (fs-CARS) with femtosecond laser pulses detected in the near-field using SNOM. We demonstrate that highly spatially resolved images can be obtained from poly(3-hexylthiophene) (P3HT) nano-structures where the fs-CARS process was in resonance with the P3HT absorption and with characteristic P3HT vibrational modes without destruction of the samples. Sub-diffraction limited lateral resolution is achieved. Especially the height resolution clearly surpasses that obtained with standard microCARS. These results will be the basis for future investigations of mode-selective dynamics in the near-field.

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Section: Figure 10contrasting

confidence: 59%

“…Surface enhancement of CARS was observed experimentally by Liang et al using a nanosecond laser [44]. In their experiment, samples used were organic solvents, such as benzene and toluene adsorbed onto colloidal silver particles prepared in N,N-dimethylformamide.…”

Section: Figure 10mentioning

confidence: 97%

Nonlinear spectroscopy in the near-field: time resolved spectroscopy and subwavelength resolution non-invasive imaging

et al. 2014

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“…7 It was demonstrated that even nonlinear Raman spectroscopy is strongly influenced by the surface enhancement effect. 8 Theoretical methods used to explain Raman spectra only partly explain the SERS spectra. 9 This is due to the complicated mechanisms responsible for the excitation of the scattering process.…”

Section: Introductionmentioning

confidence: 99%

Surface enhanced Raman scattering (SERS)—a quantitative analytical tool?

Sackmann

Materny

2006

J Raman Spectroscopy

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145

113

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Raman spectroscopy is a widely used analytical tool capable of providing valuable information about the chemical structure and composition of molecules. In order to detect substances also at a very low concentration levels, Surface Enhanced Raman Scattering (SERS) was introduced. The different amplification mechanisms result in extreme sensitivity, however, a quantitative use of SERS appears to be problematic. Especially, when deploying silver sols as SERS substrates, the reproducibility of the signal intensities for a given substance concentration is questionable. Experimental results of an investigation of this problem for low concentrations of adenine are presented. Comparison with results obtained for different SERS substrates by other authors reveals clearly different dependencies. Only in a very limited concentration range reproducible and therefore quantitatively utilizable data could be obtained.

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“…If the input (o P , o S ) or output (o AS ) frequencies in CARS are in resonance with the collective modes of the plasmonic nanostructure, the surface-enhanced CARS (SECARS) [18][19][20][21] signal from molecules adsorbed onto the nanostructure will be further enhanced by the local fields of the excited plasmon modes. The EM enhancement factor in SECARS is given by…”

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confidence: 99%

Coherent anti-Stokes Raman scattering with single-molecule sensitivity using a plasmonic Fano resonance

et al. 2014

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Plasmonic nanostructures are of particular interest as substrates for the spectroscopic detection and identification of individual molecules. Single-molecule sensitivity Raman detection has been achieved by combining resonant molecular excitation with large electromagnetic field enhancements experienced by a molecule associated with an interparticle junction. Detection of molecules with extremely small Raman cross-sections (B10 À 30 cm 2 sr À 1 ), however, has remained elusive. Here we show that coherent anti-Stokes Raman spectroscopy (CARS), a nonlinear spectroscopy of great utility and potential for molecular sensing, can be used to obtain single-molecule detection sensitivity, by exploiting the unique light harvesting properties of plasmonic Fano resonances. The CARS signal is enhanced by B11 orders of magnitude relative to spontaneous Raman scattering, enabling the detection of single molecules, which is verified using a statistically rigorous bi-analyte method. This approach combines unprecedented single-molecule spectral sensitivity with plasmonic substrates that can be fabricated using top-down lithographic strategies.

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Experimental observation of surface-enhanced coherent anti-Stokes Raman scattering

Cited by 77 publications

References 18 publications

Nonlinear spectroscopy in the near-field: time resolved spectroscopy and subwavelength resolution non-invasive imaging

Nonlinear spectroscopy in the near-field: time resolved spectroscopy and subwavelength resolution non-invasive imaging

Surface enhanced Raman scattering (SERS)—a quantitative analytical tool?

Coherent anti-Stokes Raman scattering with single-molecule sensitivity using a plasmonic Fano resonance

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