Tip-Enhanced Raman Excitation Spectroscopy (TERES):
Direct Spectral Characterization of the Gap-Mode Plasmon
Posted on 2019-09-17 - 20:46
The
plasmonic properties of tip–substrate composite systems
are of vital importance to near-field optical spectroscopy, in particular
tip-enhanced Raman spectroscopy (TERS), which enables operando studies
of nanoscale chemistry at a single molecule level. The nanocavities
formed in the tip–substrate junction also offer a highly tunable
platform for studying field-matter interactions at the nanoscale.
While the coupled nanoparticle dimer model offers a correct qualitative
description of gap-mode plasmon effects, it ignores the full spectrum
of multipolar tip plasmon modes and their interaction with surface
plasmon polariton (SPP) excitation in the substrate. Herein, we perform
the first tip-enhanced Raman excitation spectroscopy (TERES) experiment
and use the results, both in ambient and aqueous media, in combination
with electrodynamics simulations, to explore the plasmonic response
of a Au tip–Au substrate composite system. The gap-mode plasmon
features a wide spectral window corresponding to a host of tip plasmon
modes interacting with the plasmonic substrate. Simulations of the
electric field confinement demonstrate that optimal spatial resolution
is achieved when a hybrid plasmon mode that combines a multipolar
tip plasmon and a substrate SPP is excited. Nevertheless, a wide spectral
window over 1000 nm is available for exciting the tip plasmon with
high spatial resolution, which enables the simultaneous resonant detection
of different molecular species. This window is robust as a function
of tip–substrate distance and tip radius of curvature, indicating
that many choices of tips will work, but it is restricted to wavelengths
longer than ∼600 nm for the Au tip–Au substrate combination.
Other combinations, such as Ag tip–Ag substrate, can access
wavelengths as low as 350 nm.
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Yang, Muwen; Mattei, Michael S.; Cherqui, Charles R.; Chen, Xu; Van Duyne, Richard P.; Schatz, George C. (2019). Tip-Enhanced Raman Excitation Spectroscopy (TERES):
Direct Spectral Characterization of the Gap-Mode Plasmon. ACS Publications. Collection. https://doi.org/10.1021/acs.nanolett.9b02925
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AUTHORS (6)
MY
Muwen Yang
MM
Michael S. Mattei
CC
Charles R. Cherqui
XC
Xu Chen
RV
Richard P. Van Duyne
GS
George C. Schatz
KEYWORDS
field-matter interactionsgap-mode plasmon featuresnanoparticle dimer modelmolecule leveltip-enhanced Raman spectroscopytip radiusplasmonic responsemultipolar tip plasmonSpectral Characterizationfield confinementtip plasmongap-mode plasmon effectsOther combinationsTEREStunable platformsubstrate SPPmultipolar tip plasmon modestip-enhanced Raman excitation spectroscopyplasmonic substrate350 nmplasmonic propertiessurface plasmon polaritonnanoscale chemistrytip plasmon modes1000 nmTip-Enhanced Raman Excitation SpectroscopyGap-Mode PlasmonTERSplasmon modeelectrodynamics simulationsoperando studies