Surface-enhanced femtosecond CARS spectroscopy (SE-CARS) on pyridine

Namboodiri, V.; Namboodiri, M.N.; Diaz, G.I. Cava; Oppermann, Malte; Flachenecker, G.; Materny, Arnulf

doi:10.1016/j.vibspec.2010.08.005

Cited by 37 publications

(30 citation statements)

References 12 publications

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“…Thus the polarizability gradients responsible for resonant signal should approximately depend on the electronic structure only near the small molecule, and our DFT/TDDFT approach can be used to examine chemical enhancement of CARS. A CARS experiment for pyridine on silver colloid has been recently published 42 which reports a 10x CARS signal enhancement, and a SERS enhancement of 10 4 . Cluster models have been systemically investigated 43 for simulating the chemical portion of the enhancement.…”

Section: Surface Effectsmentioning

confidence: 99%

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Parkhill

Rappoport

Aspuru‐Guzik

2011

J. Phys. Chem. Lett.

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We present the first density functional simulations of coherent anti-Stokes Raman scattering (CARS) and an analysis of the chemical effects upon binding to a metal surface. Spectra are obtained from first-principles electronic structure calculations and are compared with available experiments and previously available theoretical results following from Hartree–Fock polarizability derivatives. A first approximation to the nonresonant portion of the CARS signal is also explored. We examine the silver pyridine cluster models of the surface chemical signal enhancement, previously introduced for surface-enhanced Raman scattering. Chemical resonant intensity enhancements of roughly 102 are found for several model clusters. The prospects of realizing further enhancement of CARS signal with metal surfaces is discussed in light of the predicted chemical enhancements.

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Section: Surface Effectsmentioning

confidence: 99%

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Parkhill

Rappoport

Aspuru‐Guzik

2011

J. Phys. Chem. Lett.

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“…Both the forward directed signal and 90° scattered signal are detected. In the femtosecond experiments only the forward directed (phase matched) signal could be observed [15].…”

Section: Pump-probe Scanning Near-field Microscopy (Pp-snom)mentioning

confidence: 99%

“…The CARS signal detected in the forward direction was weaker, which was explained to be due to the scattering of the signal by the silver particles. The work described here is an extension of this experiment using femtosecond pulses and is aimed at understanding the mechanism of enhancement of the CARS signal from molecules adsorbed onto colloidal nanoparticles of coin metals, such as silver and gold [15]. Recently, there has been a number of reports on SE-CARS.…”

Section: Figure 10mentioning

confidence: 99%

“…The principle preparation technique (detailed in ref. 15), temperature and light conditions, speed of addition of reagents for the preparation of colloids etc. affect the SERS activity of the colloids.…”

Section: Figure 10mentioning

confidence: 99%

“…In the following, we would like to review some of our own works, which already have been published elsewhere [8,14,15]. Besides this, the review will also give an insight into the state of art in the field of nonlinear optical spectroscopy with sub-diffraction limited spatial resolution.…”

Section: Introductionmentioning

confidence: 99%

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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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Surface‐EnhancedRaman Scattering of Biological Materials

Todorović

Murgida

2016

Encyclopedia of Analytical Chemistry

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Surface‐enhanced Raman spectroscopy (SERS) is a very powerful vibrational method that can be applied to a variety of biological samples provided that drawbacks, such as poor reproducibility of the signal and biocompatibility of the substrates, can be satisfactorily overcome. SERS is characterized by very low limits of detection, mainly due to the electromagnetic enhancement of the Raman signals, capable of achieving the single‐molecule level. Moreover, the spectra of small molecules represent authentic molecular fingerprints with very narrow linewidths that, along with the additional enhancement and inter‐/intramolecular selectivity gained through resonant laser excitation (surface‐enhanced resonance Raman spectroscopy, SERRS), make this technique particularly suited for multiplexing applications in complex biological samples. In this article, we introduce first the physical principles of SER(R)RS and describe the different types of substrates, as well as the basic modern instrumentation. We then provide an overview of recent biological applications, including biophysical mechanistic and structural studies on isolated biomolecules, their direct and indirect detection, chemical imaging of biological samples, and biomedical applications. Finally, we briefly discuss our outlook for the future research in this field.

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Surface-enhanced femtosecond CARS spectroscopy (SE-CARS) on pyridine

Cited by 37 publications

References 12 publications

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

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

Surface‐EnhancedRaman Scattering of Biological Materials

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