Single-molecule (SM) surface-enhanced Raman spectroscopy (SERS) and tip-enhanced Raman spectroscopy (TERS) have emerged as analytical techniques for characterizing molecular systems in nanoscale environments. SERS and TERS use plasmonically enhanced Raman scattering to characterize the chemical information on single molecules. Additionally, TERS can image single molecules with subnanometer spatial resolution. In this review, we cover the development and history of SERS and TERS, including the concept of SERS hot spots and the plasmonic nanostructures necessary for SM detection, the past and current methodologies for verifying SMSERS, and investigations into understanding the signal heterogeneities observed with SMSERS. Moving on to TERS, we cover tip fabrication and the physical origins of the subnanometer spatial resolution. Then, we highlight recent advances of SMSERS and TERS in fields such as electrochemistry, catalysis, and SM electronics, which all benefit from the vibrational characterization of si...

Single-Molecule Chemistry with Surface- and Tip-Enhanced Raman Spectroscopy

Driven by applications in chemical sensing, biological imaging and material characterisation, Raman spectroscopies are attracting growing interest from a variety of scientific disciplines The Raman effect originates from the inelastic scattering of light, and it can directly probe vibration/rotational-vibration states in molecules and materials Despite numerous advantages over infrared spectroscopy, spontaneous Raman scattering is very weak, and consequently, a variety of enhanced Raman spectroscopic techniques have emerged These techniques include stimulated Raman scattering and coherent anti-Stokes Raman scattering, as well as surface- and tip-enhanced Raman scattering spectroscopies The present review provides the reader with an understanding of the fundamental physics that govern the Raman effect and its advantages, limitations and applications The review also highlights the key experimental considerations for implementing the main experimental Raman spectroscopic techniques The relevant data analysis methods and some of the most recent advances related to the Raman effect are finally presented This review constitutes a practical introduction to the science of Raman spectroscopy; it also highlights recent and promising directions of future research developments

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Raman Techniques: Fundamentals and Frontiers

This review discusses a relatively new technique for optical nanoimaging at visible wavelength, known as tip-enhanced Raman spectroscopy (TERS). This technique relies on the enhancement and spatial confinement of light in the close vicinity of the apex of a plasmonic nanotip. The plasmonic nanotip can be positioned on the sample and controlled by a suitable scanning probe microscopy, such as atomic force microscopy or scanning tunneling microscopy. By raster scanning the nanotip, one can obtain nanoimages with high spatial resolution. While enhancement helps measuring weak phonon modes from a tiny volume of the sample, confinement delivers extremely high spatial resolution in nanoimaging. We will discuss the technique of TERS in more detail with several applications and review the recent advances.

Tip-Enhanced Raman Spectroscopy: Technique and Recent Advances.

Tip-enhanced Raman spectroscopy (TERS) is a very powerful variant of surface-enhanced Raman spectroscopy (SERS). In a sense, TERS overcomes most of the drawbacks of SERS but keeps its advantages, such as its high sensitivity. TERS offers the additional advantages of high spatial resolution, much beyond the Abbe limit, and the possibility to correlate TER and other scanning probe microscope images, i.e., to correlate topographic and chemical data. TERS finds application in a number of fields, such as surface science, material science, and biology. Single-molecule TERS has been observed even for TERS enhancements of “only” 10 6 –10 7 . In this review, TERS enhancements are discussed in some detail, including a condensed overview of measured contrasts and estimated total enhancements. Finally, recent developments for TERS under ultrahigh vacuum conditions are presented, including TERS on a C60 island with a diameter of a few tens of nanometers, deposited on a smooth Au(111) surface.

/pdf/tip-enhanced-raman-spectroscopy-near-fields-acting-on-a-few-24tfl8amet.pdf

Tip-enhanced Raman spectroscopy: near-fields acting on a few molecules.

Methods for chemical analysis at the nanometer scale are crucial for understanding and characterizing nanostructures of modern materials and biological systems. Tip-enhanced Raman spectroscopy (TERS) combines the chemical information provided by Raman spectroscopy with the signal enhancement known from surface-enhanced Raman scattering (SERS) and the high spatial resolution of atomic force microscopy (AFM) or scanning tunneling microscopy (STM). A metallic or metallized tip is illuminated by a focused laser beam and the resulting strongly enhanced electromagnetic field at the tip apex acts as a highly confined light source for Raman spectroscopic measurements. This Review focuses on the prerequisites for the efficient coupling of light to the tip as well as the shortcomings and pitfalls that have to be considered for TERS imaging, a fascinating but still challenging way to look at the nanoworld. Finally, examples from recent publications have been selected to demonstrate the potential of this technique for chemical imaging with a spatial resolution of approximately 10 nm and sensitivity down to the single-molecule level for applications ranging from materials sciences to life sciences.

Nanoscale chemical imaging using tip-enhanced Raman spectroscopy: a critical review.

A versatile and efficient tip-enhanced spectroscopic imaging technique based on a parabolic mirror (PM) assisted near-field optical microscope is demonstrated. The replacement of the conventional objective lens with a parabolic mirror allows the non-restricted investigation of sample materials regarding their opacity. In addition, an improved signal collection efficiency and effective excitation of the longitudinal plasmonic oscillation in the tip apex are obtained. The capabilities of PM-assisted tip-enhanced Raman (TER) and photoluminescence (PL) imaging in distinguishing the individual domains made of different chemical components in poly (3-hexythiophene)/[6, 6]-penyl-C61 butyric acid methyl ester (P3HT/PCBM) solar cell blend film and in the investigation of the plasmonic properties of geometrically well-defined Au cones are demonstrated. Copyright © 2009 John Wiley & Sons, Ltd.

Parabolic mirror‐assisted tip‐enhanced spectroscopic imaging for non‐transparent materials

Regular arrays of metallic nano-triangles – so called Fischer patterns – are fabricated by nano-sphere lithography. We studied such gold nano-triangle arrays on silicon or glass substrates. A series of different samples was investigated with a parabolic mirror based confocal microscope where the sample is scanned through the laser focus. By employing higher order laser modes (azimuthally and radially polarised laser beams), we can excite the Fischer patterns using either a pure in-plane (x,y) electric field or a strongly z-directional (optical axis of the optical microscope) electric field. We collected and evaluated the emitted luminescence and thereby investigated the respectively excited plasmonic modes. These varied considerably: firstly with the light polarisation in the focus, secondly with the aspect ratio of the triangles and thirdly with the employed substrate. Moreover, we obtained strongly enhanced Raman spectra of an adenine (sub-)monolayer on gold Fischer patterns on glass. We thus showed that gold Fischer patterns are promising surface-enhanced Raman scattering (SERS) substrates.

/pdf/assessing-the-plasmonics-of-gold-nano-triangles-with-higher-wonz8hva0b.pdf

Assessing the plasmonics of gold nano-triangles with higher order laser modes.

Calf thymus DNA adsorbed on a rough gold substrate or on an atomically smooth gold (111) surface has been investigated by collecting its unique Raman fingerprints using either surface-enhanced Raman scattering (SERS) or tip-enhanced Raman scattering (TERS). A monolayer coverage of DNA strands adsorbed at both the irregular rough edges of evaporated gold grids and at gold nanoparticles is detected by SERS. Highly improved sensitivity down to single DNA strand spectroscopic determination is accomplished by TERS providing an enhancement factor of at least 1400. Based on our experimental results, we propose that TERS is a promising technique to study the DNA–drug molecule interaction on the level of a single DNA strand.

/pdf/surface-and-tip-enhanced-raman-spectroscopy-of-dna-2cfa8qzvq4.pdf

Surface- and tip-enhanced Raman spectroscopy of DNA

Tip-enhanced near-field optical images and correlated topographic images of an organic semiconductor film (diindenoperylene, DIP) on Si have been recorded with high optical contrast and high spatial resolution (17 nm) using a parabolic mirror with a high numerical aperture for tip illumination and signal collection. The DIP molecular domain boundaries being one to four molecular layers (1.5-6 nm) high are resolved topographically by a shear-force scanning tip and optically by simultaneously recording the 6 × 10 5 times enhanced photoluminescence (PL). The excitation is 4 × 10 4 times enhanced and the intrinsically weak PL-yield of the DIP-film is 15-fold enhanced by the tip. The Raman spectra indicate an upright orientation of the DIP molecules. The enhanced PL contrast results from the local film morphology via stronger coupling between the tip plasmon and the exciton-polariton in the DIP film.

/pdf/nanoscale-spectroscopic-imaging-of-organic-semiconductor-2jv8ihn484.pdf

Nanoscale spectroscopic imaging of organic semiconductor films by plasmon-polariton coupling.

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Parabolic mirror‐assisted tip‐enhanced spectroscopic imaging for non‐transparent materials

Assessing the plasmonics of gold nano-triangles with higher order laser modes.

Surface- and tip-enhanced Raman spectroscopy of DNA

Nanoscale spectroscopic imaging of organic semiconductor films by plasmon-polariton coupling.