The properties of a surface have crucial roles in deter-
mining its adhesion, friction, wear and wetting behav-
iour, as well as surface chemical processes such as
catalysis, corrosion, sintering, composite formation and
electrochemistry
1,2
. With the development of surface
engineering techniques and nanotechnology, research
has shifted from homogeneous to composite materials,
from almost perfect single-crystal surfaces to surfaces
with functionalized ‘active sites’, and from thin-film
materials to promising 2D materials with one to several
atomic layers in thickness. Meanwhile, characterization
techniques have been developed to reveal the struc-
ture–property relationships of these emerging materials.
However, for most techniques, the signals obtained from
the surfaces are either too weak to detect or are difficult
to resolve into distinct components because of the low
spectral and spatial resolution. Therefore, it is necessary
to develop in situ techniques with ultrahigh sensitivity,
surface specificity, high spectral resolution, and high
spatial and temporal resolution.
One such technique is surface-enhanced Raman
spectroscopy (SERS)
3–5
, which can realize an ultrahigh
sensitivity down to the single-molecule level by means
of coinage-metal (for example, Au, Ag and Cu) nano-
structures
6,7
. The SERS effect is due to the amplification
of Raman signals of analytes by several orders of magni-
tude when the analytes are located at or very close to
coinage-metal nanostructures (the working princi-
ples of SERS are described in BOXES 1,2)
8
. The SERS
enhancement of these nanostructures strongly relies
on the optical resonance properties of coinage-metal
nanostructures, which can significantly enhance the
local electromagnetic field, largely owing to the excita-
tion of surface plasmon resonance (SPR)
9,10
. Based on
similar surface-enhancement mechanisms, many other
surface-enhanced Raman methods, including the two
important variants of SERS — tip-enhanced Raman
spectroscopy (TERS)
11–14
and shell-isolated nanoparticle-
enhanced Raman spectroscopy (SHINERS)
15
— as
well as ultraviolet SERS, near-infrared SERS
16–18
and
surface-enhanced nonlinear Raman spectroscopy
19–22
,
have been developed for a wide range of applications.
The above-mentioned techniques can be collectively
described as plasmon-enhanced Raman spectroscopy
(PERS)
23
(a timeline of the key developments of PERS
techniques is provided in FIG. 1).
PERS enhancement is strongly dependent on the opti-
cal properties, shape and aggregation of nanomaterials
24
.
In the 1970s and 1980s, SERS-active substrates, such as
roughened Au and Ag electrodes, colloidal aggregates
1
State Key Laboratory for
Physical Chemistry of Solid
Surfaces, College of
Chemistry and Chemical
Engineering, iChEM, Xiamen
University.
2
MOE Key Laboratory of
Spectrochemical Analysis and
Instrumentation, Xiamen
University, Xiamen 361005,
China.
Correspondence to Z-.Q.T.
zqtian@xmu.edu.cn
Article number: 16021
doi:10.1038/natrevmats.2016.21
Published online 26 Apr 2016
Nanostructure-based plasmon-
enhanced Raman spectroscopy for
surface analysis of materials
Song-Yuan Ding
1
, Jun Yi
1
, Jian-Feng Li
1,2
, Bin Ren
1,2
, De-Yin Wu
1
,
Rajapandiyan Panneerselvam
1
and Zhong-Qun Tian
1
Abstract | Since 2000, there has been an explosion of activity in the field of plasmon-enhanced
Raman spectroscopy (PERS), including surface-enhanced Raman spectroscopy (SERS),
tip-enhanced Raman spectroscopy (TERS) and shell-isolated nanoparticle-enhanced Raman
spectroscopy (SHINERS). In this Review, we explore the mechanism of PERS and discuss PERS
hotspots — nanoscale regions with a strongly enhanced local electromagnetic field — that
allow trace-molecule detection, biomolecule analysis and surface characterization of various
materials. In particular, we discuss a new generation of hotspots that are generated from hybrid
structures combining PERS-active nanostructures and probe materials, which feature a strong
local electromagnetic field on the surface of the probe material. Enhancement of surface
Raman signals up to five orders of magnitude can be obtained from materials that are weakly
SERS active or SERS inactive. We provide a detailed overview of future research directions in
the field of PERS, focusing on new PERS-active nanomaterials and nanostructures and the
broad application prospect for materials science and technology.
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