Chemical mapping of a single molecule by plasmon-enhanced Raman scattering

  title={Chemical mapping of a single molecule by plasmon-enhanced Raman scattering},
  author={R. Zhang and Y. Q. Zhang and Zhenchao Dong and Shaolong Jiang and C. Zhang and L G Chen and L. D. Zhang and Yuan Liao and Javier Aizpurua and Y Luo and J. L. Yang and J. G. Hou},
Visualizing individual molecules with chemical recognition is a longstanding target in catalysis, molecular nanotechnology and biotechnology. Molecular vibrations provide a valuable ‘fingerprint’ for such identification. Vibrational spectroscopy based on tip-enhanced Raman scattering allows us to access the spectral signals of molecular species very efficiently via the strong localized plasmonic fields produced at the tip apex. However, the best spatial resolution of the tip-enhanced Raman… 
Distinguishing adjacent molecules on a surface using plasmon-enhanced Raman scattering.
Two different adjacent molecules that are within van der Waals contact and of very similar chemical structure on a silver surface can be distinguished in real space using a nonlinear scanning tunnelling microscope-controlled TERS set-up.
Single-molecule resonance Raman effect in a plasmonic nanocavity
Investigation of an isolated copper naphthalocyanine molecule adsorbed on a triple-layer NaCl on Ag(111) using scanning tunnelling microscope TERS imaging reveals components of the electric field perpendicular to the tip provide sensitivity to the symmetry of the vibrational modes of the molecule.
Single-Molecule Imaging Using Atomistic Near-Field Tip-Enhanced Raman Spectroscopy.
A systematic theoretical study of TERS imaging of single molecules, using a hybrid atomistic electrodynamics-quantum mechanical method, which provides insights into single-molecule imaging based on TERS and Raman scattering of molecules in nanojunctions with atomic dimensions.
Coherent anti-Stokes Raman scattering with single-molecule sensitivity using a plasmonic Fano resonance.
It is shown that coherent anti-Stokes Raman spectroscopy (CARS) can be used to obtain single-molecule detection sensitivity, by exploiting the unique light harvesting properties of plasmonic Fano resonances.
Theoretical Modeling of Plasmon-Enhanced Raman Images of a Single Molecule with Subnanometer Resolution.
A quantum-mechanical description of the interaction between a molecule and a highly confined plasmonic field is reported and the present theory provides the basic framework for describing linear and nonlinear responses of molecules underhighly confined plAsmonic fields.
Tip enhanced Raman scattering: plasmonic enhancements for nanoscale chemical analysis
Abstract Tip enhanced Raman scattering (TERS) is an emerging technique that uses a metalized scanning probe microscope tip to spatially localize electric fields that enhances Raman scattering
Single-Molecule Chemistry with Surface- and Tip-Enhanced Raman Spectroscopy.
This review of single-molecule surface-enhanced Raman spectroscopy and TERS covers the development and history, 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.
Molecular cavity optomechanics as a theory of plasmon-enhanced Raman scattering.
The optomechanical approach recovers known results, provides a quantitative framework for the calculation of cross-sections, and enables the design of novel systems that leverage dynamical backaction to achieve additional, mode-selective enhancements.
Resolving the Correlation between Tip-Enhanced Resonance Raman Scattering and Local Electronic States with 1 nm Resolution
This work reports on tip-enhanced resonance Raman spectroscopy (TERRS) of ultrathin ZnO layers epitaxially grown on a Ag(111) surface, and suggests that TERRS is a new approach for the atomic-scale optical characterization of local electronic states at near-atomic resolution.
Visualizing vibrational normal modes of a single molecule with atomically confined light
The vibrational normal modes in a single molecule are imaged using tip-enhanced Raman spectromicroscopy performed in the atomistic near-field, and ångström-scale resolution is attained at subatomic separation between the tip atom and a molecule in the quantum tunnelling regime of plasmons.


Scanning-probe Raman spectroscopy with single-molecule sensitivity
Single-molecule spectroscopy has matured into diverse areas with its most notable contributions in the determination of biomolecular processes even under ambient or physiological conditions. 1‐4 So
Tip-enhanced Raman spectroscopy: near-fields acting on a few molecules.
In this review, TERS enhancements are discussed in some detail, including a condensed overview of measured contrasts and estimated total enhancements.
Catalytic processes monitored at the nanoscale with tip-enhanced Raman spectroscopy.
It is shown that time-resolved tip-enhanced Raman spectroscopy can monitor photocatalytic reactions at the nanoscale and can be used to observe other molecular effects such as monolayer diffusion.
Pressure-assisted tip-enhanced Raman imaging at a resolution of a few nanometres
Scanning probe microscopy methods1,2 can image samples with extremely high resolutions, opening up a wide range of applications in physics3, chemistry4 and biology5. However, these passive
Nanoscale chemical imaging using top-illumination tip-enhanced Raman spectroscopy.
For the first time, large (64 × 64 up to 200 × 200 pixels), high-resolution TERS imaging with full spectral information at every pixel is shown, which is necessary for the chemical identification of sample constituents.
Electromagnetic contributions to single-molecule sensitivity in surface-enhanced raman scattering
  • C. Xu, Aizpurua, Kall, Apell
  • Chemistry
    Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics
  • 2000
The calculations indicate that the maximum enhancement factor achievable through electromagnetics is of the order 10(11), which can qualitatively explain why only very few surface sites seem to contribute to the measured signal in single-molecule SERS experiments.
Single-Molecule Tip-Enhanced Raman Spectroscopy
An existence proof for single-molecule tip-enhanced Raman spectroscopy (SMTERS) is given using the frequency domain approach involving the two isotopologues of Rhodamine 6G (R6G) that were previously
Revealing the molecular structure of single-molecule junctions in different conductance states by fishing-mode tip-enhanced Raman spectroscopy
Density functional theory calculations reveal that the most significant spectral change seen for a gold-4,4′-bipyridine-gold junction results from the deformation of the pyridine ring in contact with the drain electrode at high voltage, and these calculations suggest that a stronger bonding interaction between the molecule and the drain may account for the nonlinear dependence of conductance on bias voltage.
Nanoscale vibrational analysis of single-walled carbon nanotubes.
Near-field Raman imaging and spectroscopy is used to study localized vibrational modes along individual, single-walled carbon nanotubes (SWNTs) and finds that for arc-discharge SWNTs, both the radial breathing mode (RBM) and intermediate frequency mode (IFM) are highly localized.