Sensors 2011, 11, 10907-10929; doi:10.

3390/s111110907
OPEN ACCESS

sensors
ISSN 1424-8220
www.mdpi.com/journal/sensors

Review

Plasmonic Nanostructures for Nano-Scale Bio-Sensing

Taerin Chung 1, Seung-Yeol Lee 1, Eui Young Song 1, Honggu Chun 2 and Byoungho Lee 1,*
1
National Creative Research Center for Active Plasmonics Application Systems, Inter-University
Semiconductor Research Center and School of Electrical Engineering, Seoul National University,
Gwanak-Gu Gwanakro 1, Seoul 151-744, Korea; E-Mails: [email protected] (T.C.);
[email protected] (S.-Y.L.); [email protected] (E.Y.S.)
2
Department of Biomedical Engineering, Korea University, Seoul 136-701, Korea;
E-Mail: [email protected]

* Author to whom correspondence should be addressed; E-Mail: [email protected];

Tel.: +82-2-880-7245; Fax: +82-2-873-9953.

Received: 8 October 2011; in revised form: 13 November 2011 / Accepted: 14 November 2011 /
Published: 21 November 2011

Abstract: The optical properties of various nanostructures have been widely adopted for
biological detection, from DNA sequencing to nano-scale single molecule biological
function measurements. In particular, by employing localized surface plasmon resonance
(LSPR), we can expect distinguished sensing performance with high sensitivity and
resolution. This indicates that nano-scale detections can be realized by using the shift of
resonance wavelength of LSPR in response to the refractive index change. In this paper, we
overview various plasmonic nanostructures as potential sensing components. The qualitative
descriptions of plasmonic nanostructures are supported by the physical phenomena such as
plasmonic hybridization and Fano resonance. We present guidelines for designing specific
nanostructures with regard to wavelength range and target sensing materials.

Keywords: surface plasmon resonance; optical sensors; plasmonic sensors; nanostructure

1. Introduction

As nano-fabrication processes have rapidly developed, the recent sensor technologies are being used
for reading DNA bases [1] as well as detecting protein-protein interactions [2,3], surface membrane
binding events [4] and antigen-antibody recognition events [5]. In particular, the demand for surface
Sensors 2011, 11 10908

plasmon resonance (SPR)-based nano-scale bio-sensing has increased due to the advantage of
label-free, minimal interference, and real-time monitoring performance [6]. The conventional SPR
sensor originates from propagating surface plasmons. This plasmon can be described as surface
plasmon polaritons in optically thin metal film, usually noble metal layers. Propagating plasmon waves
can be produced in various illumination configurations from grating coupling to near-field excitation.
The universal scheme for SPR sensing is the Kretschmann geometry where a thin noble metal film is
covered on a prism. However, it has drawbacks in applications due to its bulky system and low spectral
resolution [7,8]. On the other hand, localized SPR (LSPR), a coupling between electromagnetic field and
spatially confined free-electrons, has a potential for resolving these issues in an attempt to detect
nano-scale biological interactions. LSPR sensing structures are typically fabricated on a chip where
noble metal nanostructures are coated or patterned on a dielectric substrate. It seems feasible that
sensor system can be miniaturized by nano-scaled localized plasmons installed on effectual
microspectroscopy. Since the resonance condition of LSPR is determined by the electron motions,
optical properties of this sensing scheme are highly dependent on the geometry of metallic nanostructures.
Such nanostructures for achieving LSPR can resonate with the incidence of electromagnetic fields at
certain wavelengths, giving rise to strongly enhanced near-fields [9,10]. Plasmon excitations on the
metallic nanostructures can be a promising constituent of the propagating plasmon employed in
traditional SPR sensors. As compared to SPR sensors, LSPR sensors can be advantageous due to their
capability of optimizing the sensing performance through variations of the size and shapes of
nanostructures. The extremely intense and highly confined electromagnetic fields induced by the LSPR
can realize a highly sensitive probe to detect small changes in the dielectric environment around the
nanostructures. When the biomolecular binding events get close to the surface of a noble metal
nanostructure, the refractive index of immediate environment surrounding the nanostructure is
increased. Thus, biomolecular interactions at the surface of the nanostructures directly lead to local
refractive index changes; these changes can then be monitored via the LSPR peak wavelength shift.
This can allow for the detection of extremely low concentrations of molecules with surface-enhanced
Raman scattering (SERS) [11,12] as well. Hence, the ideal LSPR nanosensor should have a high
spectral shift along the alteration of surrounding material and a narrow linewidth of spectral response [13].
Yet, lower sensitivity has been marked at LSPR sensors compared with their counterparts.
Major issues of current LSPR bio-sensor research include understanding LSPR properties in certain
nanostructures, optimizing the design of nanostructures, and improving sensitivity and detection limits.
In this review, the uses of assorted nanostructures as potential sensing components are presented and
re-categorized according to their similar characteristics. Exemplary cases of biological sensing with
LSPR are addressed.

2. Basic Principle of Localized Surface Plasmon Resonance

When a metallic nanostructure is illuminated by an appropriate incident wavelength, localized

electrons in the metallic nanostructure oscillate and create strong surface waves [14]. The curved
surface of the particle generates an effective restoring force on the conduction electrons so that
resonance can arise. This phenomenon leads to strong field enhancement in the near field zone. This
Sensors 2011, 11 10909

resonance is called LSPR. The LSPR phenomenon is theoretically possible in any kind of metal,
semiconductor or alloy with a large negative real part and small imaginary part of electric permittivity.
We can obtain the explicit form of electromagnetic field distribution using some assumptions when
a particle interacts with electromagnetic field. First, we assume the particle size is much smaller than
wavelength of light in the surrounding medium. In this condition, the phase of the harmonically
oscillating electromagnetic field is approximately constant over the particle volume. This is called
quasi-static approximation. Second, we choose a simple geometry for analytical treatment: The particle
is a homogeneous isotropic sphere of radius r0, and surrounding material is a homogeneous, isotropic
and non-absorbing medium. On the illumination of static electric fields, we solve Laplace equation for
the potential, ∇ 2V =0 . Due to the azimuthal symmetry of the problem and requirement that the
potentials remain finite at the center of the particle, the solutions of this Laplace equation for potentials
inside and outside the particle can be written as:
∞
Vin (r,θ ) = ∑ Al r l Pl (cosθ ),
l =0
∞ (1)
Vout (r,θ ) = ∑  Bl r l + Cl r −(l +1)  Pl (cosθ ).
l =0

where, Pl(cosθ) is the Legendre polynomial of order l, and θ is the angle between the position vector r

and the electric field E . The coefficients Al, Bl, Cl can be determined using boundary conditions: as r

approaches infinity, the potential approaches –| E | rcosθ. The tangential components of electric fields
are equal at r = r0, and normal components of electric flux density are equal at r = r0. The solutions
are:
3ε d 
Vin = − E r cosθ ,
ε m (ω ) + 2ε d
 ε (ω ) - ε d  3 cosθ (2)
Vout =− E r cosθ + m E r0 2 .
ε m (ω ) + 2ε d r
Here, εm(ω) and εd are electric permittivity of metal and surrounding dielectric layer, respectively.
We can interpret Vout physically: Vout is the superposition of the applied field and a dipole induced

by this field. Therefore, we introduce the dipole moment p as:
 ε (ω ) - ε d 
p = 4πε 0ε d r03 m E.
ε m (ω ) + 2ε d (3)
 
If we introduce polarizability α via p = ε 0ε dα E , we can express α as:

(4)
We can expand Equation (4) in case of arbitrary shaped particle as [10]:
ε m (ω ) - ε d
α = (1 + κ )εΩ . (5)
ε m (ω ) + κε d
where Ω is the volume of the particle. As can be seen, the dipolar polarizability α could be maximized
at the condition of Re(εm(ω)) = −кεd, which is denoted by the resonance condition of LSPR assuming
Im(εm(ω)) is relatively small and constant value with the variation of frequency. к is a shape factor that
embodies geometrical polarizability of the surface that indicates the electron oscillations. The shape
factor of a small nanostructure plays a critical role to increase dipolar polarizability for enhancing
LSPR strength. This variable can be straightforwardly expressed by aspect ratio [15]. In other words,
Sensors 2011, 11 10910

resonant enhancement increases as particles are made more needle-like. A nanorod is designed for
achieving higher aspect ratio in that dipolar polarizability linearly depends on the aspect ratio of a
nanostructure. The notable increase of aspect ratio can lead to the sensitivity improvement
accompanied by remarkable wavelength shift [16].

3. Design Principles for LSPR Sensing

In this section, we will introduce the various principles for designing the highly sensitive and
strongly enhanced LSPR sensors. In attempt to compare sensing performance, several major factors
such as sensitivity, figure of merit (FOM) and resolution will be introduced.
First of all, sensitivity S is defined as the ratio of resonant wavelength shift ∂λ res to the variation of
surrounding refractive index ∂ns :
∂λ res (nm)
S= , (6)
∂ns ( RIU )
where RIU means refractive index unit. FOM is considered as a useful parameter in verifying LSPR
nanosensor. It is defined as the ratio of the refractive index sensitivity to the resonance width Δλ:
S (nm ⋅ RIU −1 )
FOM = . (7)
∆λ (nm)

Resolution is typically defined as the minimum detection limit. Unlike the conventional propagating
SPP-based sensors, localized SPPs have their own resolution for detecting the signals. This can be
improved by the size and geometry of nanostructure. These factors can describe the sensing
performance and be used in evaluating various types of sensors. Many groups have exploited various
nanostructures in attempt to improve LSPR sensor with regard to high sensitivity, FOM and spectral
resolution.

3.1. The Use of Inter-Coupling between Nanoparticles

One of the earliest LSPR sensor nanostructures was the simple sphere-shaped nanoparticle which
has the shape factor of 2. Figure 1(a) presents the localized surface plasmon field induced by a single
nanoparticle. However, it shows that the field strength is too weak and field distribution is not confined
to certain point so that it does not seem to be appropriate for detecting small volumes of bio-molecules.
Otherwise, additional field enhancement can be achieved by inter-coupling between particles when
nanoparticles are close to each other. From the inter-coupling between two nanoparticles, stronger LSPR
enhancement can be achieved based on the localized capacitive coupling at the nano gap surrounded by
nanoparticles as shown in Figure 1(b). Such LSPR enhancement originates from the charge induction
between two nanoparticles, which interact stronger as they get closer to each other. This relation
between the field enhancement factor of nanoparticle dimer and gap distance is clearly shown in
Figure 1(c). A metallic nanoparticle array has been proposed extending from this phenomenon. LSPR
sensing behaviors can be verified investigating on the resonant spectrum of metallic nanoparticle array.
The number and position of nanoparticle array is arbitrarily varied in attempt to identify the optical
resonant response.
Sensors 2011, 11 10911

Figure 1. Electric field distributions (V/m) at (a) a single Au nanoparticle and

(b) nanoparticle dimer when the incident wavelength of light is 633 nm and the magnitude
of incident electric field is 1 V/m. The diameter of Au nanoparticle is 100 nm. These
calculations are based on finite element method; (c) Field enhancement factor of
nanoparticle dimer with respect to the single nanoparticle. In all simulations in this figure,
the radius of each nanoparticle is 50 nm.

Figure 2 provides the resonant spectra of various types of nanoparticle arrays. Although LSPR
resonant wavelength is not so much shifted with the variation of the number of nanoparticles, it can be
shown that the peak of the resonance gets sharper due to the increase of particle interactions.

Figure 2. Array type of nanoparticles: (a) two nanoparticles; (b) three nanoparticles arrayed
in a transverse direction; (c) three nanoparticles arrayed in the shape of a right triangle;
(d) four nanoparticles arrayed in the shape of an isosceles triangle; (e) LSPR resonant spectra
with respect to the number and position of nanoparticles. Incident electric field is 1 V/m.
Sensors 2011, 11 10912

Figure 2. Cont.

It is also important that the shift of the resonant wavelength is negligible when the spacing interval is
higher than the diameter of nanoparticles. This uniformity characteristic is required for nanoparticle array
as a bulk refractive index sensor [17-19]. A bulk refractive index sensor has been typically characterized
by detecting the difference of surrounding refractive index.

3.2. Structural Modification for Higher Sensitivity

3.2.1. Increase of Polarizability via Multipolar Resonance

In a notable way to realize more advanced LSPR sensors, one of the useful methods is increasing
the polarizability by employing the multipolar resonance as depicted in Figure 3. Fundamentally, a
nanosphere exhibits dipolar resonance with degenerated longitudinal and transverse modes due to the
spherical symmetry. However, by the increase of aspect ratio at a nanoparticle, both transverse and
longitudinal modes are split. From these two modes, two plasmon resonant peaks are observed at
nanorods due to anisotropy [20]. Each resonant peak in two plasmon modes corresponds to
longitudinal and transverse plasmon modes, respectively. Derived from this concept, multipolar
resonances are introduced in diverse nanostructures [21]. A nanodisk displays the anisotropic property
distinct from a nanoparticle.

Figure 3. Schematic diagram for describing the polar properties of various nanostructures
that are used in LSPR sensors.

Hanarp et al. reported that the optical extinction peak as a function of refractive index is more
shifted as the aspect ratio of a nanodisk increases [22]. Figure 4 presents that optical spectrum
differently responds with regard to the aspect ratio of the nanodisk. The elongated nanodisk made by
the increase of aspect ratio shows that the resonant peak is more shifted than the resonant peak of circular
nanodisk. It can be explained that higher aspect ratio makes stronger dipole moment and acutely
Sensors 2011, 11 10913

influences on the surrounding materials. It makes the resonance more sensitive to the refractive index
changes. In addition, the magnitude of induced fields is increased due to stronger dipole moment.

Figure 4. Optical spectra in response to the variation of surrounding refractive indexes

from 1.3 to 1.5 at the nanodisk structure with respect to (a) aspect ratio 1:1 and (b) aspect
ratio 5:1. Incident electric field is 1 V/m.

High refractive index sensitivity and corresponding FOM are attributed to plasmonic nanostructures
associated with multipolar resonances. One of the representative structures which enhance its
sensitivity by increasing the polarizability is the nanocresent structure [3,23]. Adopting a sub-10 nm
sharp edge or tip, extremely high field intensity can be achieved at the nanocrescent. Localized and
confined electronmagnetic field enhancement, called “hot spot”, is attracting much attention in
designing sensors for bio-molecule detection as well. Hot spots generated at nano-scale sharp tips can
provide localized molecular sensing with the greatest sensitivity and resolution. As shown in Figure 5,
localized field intensity is much larger at the edges of a nanocrescent. The shape and dimensions of a
nanocrescent should be precisely designed to achieve localized field enhancement at the sharp edges.
One of the major physical parameters for designing a nanocrescent is the width of nanocrescent since it
strongly relates to the structural polarizability. Figure 5(a,b) show the field distribution near the
nanocrescent with the width of 50 nm, whereas Figure 5(c,d) show that of 100 nm. By comparing the
two structures, it can be shown that the local field intensity is slightly larger at the 50 nm width
nanocrescent. This can be explained by the relation between shape factor and aspect ratio, which
means that more needle-like structure can strongly enhance the field. In addition, field enhancement of
nanocrescent is strongly dependent on the polarization state of light. When illuminated by vertically
polarized light, higher field intensity can be achieved as compared with the incidence of horizontally
polarized light. This phenomenon can result from the difference of accumulated electrons at the sharp
edges of a nanocrescent. Horizontally polarized light equally separates the electrons to the both ends of
nanocrescent, whereas vertically polarized light enables electrons to totally move to sharp edges of a
nanocrescent, which leads to higher field intensity.
Moreover, some structures can be explained by the composition of both multipolar resonance and
inter-coupling of nanoparticles. For example, double nanocrescents structure facing each other is a
representative case.
Sensors 2011, 11 10914

Figure 5. Intensity distributions (arbitrary unit) of nanocrescent with respect to the width
of nanocrescent and incident polarization state of light. (a) 50 nm wide and horizontally
polarized light; (b) 50 nm wide and vertically polarized light; (c) 100 nm wide and
horizontally polarized light; (d) 100 nm wide and vertically polarized light.

As described in Figure 6, intensity distributions of double crescents are similar to the optical
responses of a single nanocrescent and sensitively respond to incident polarization of light. However,
they can produce much higher field intensity.

Figure 6. Intensity distributions (arbitrary unit) of double-crescents with respect to incident

polarization state of light: (a) vertically polarized light and (b) horizontally polarized light.
The width of a nanocrescent is fixed to 50 nm.
Sensors 2011, 11 10915

Enhanced field intensity calculated at double nanocrescents is approximately two times larger than
that of single nanocrescent for the vertically polarized case, and even higher for the horizontally
polarized case. It can support that localized capacitive inter-coupling nestled at nanogaps enhances
even more the field intensity of a single nanocrescent structure. This inter-coupling effect is more
effectively generated with horizontally polarized light, which can be explained by the attraction
between the oppositely induced charges at the end of nanocrescents.

3.2.2. The Use of Plasmon Hybridization for Enhancing LSPR Resonances

Another promising method for increasing the sensitivity of LSPR sensor is using the plasmon
hybridization [24]. Schematic diagram of representative nanostructures for LSPR sensing which is
based on plasmon hybridization is shown in Figure 7(a). Plasmon hybridization theory originates from
the hybridization of essentially fixed-frequency plasmon resonances of individual nanostructures in a
complicated nanostructure. In the model of plasmon hybridization, bonding and anti-bonding modes
are introduced. At the low energy level, bonding mode is formed by symmetrical coupling in a
nanostructure. Meanwhile, anti-bonding mode results from asymmetrical coupling in a nanostructure at
high energy level. The highly geometry-dependent plasmon response can be seen as an interaction
between two conjugated physical modes as mentioned above. The physical models of plasmonic
hybridization have been incessantly brought into novel nanostructures such as nanorings and
nanoshells. This model can be employed to take account of the sensitive geometrical tunability of the
plasmon resonant frequency of metal-based complex nanostructures [25]. The plasmon hybridization
picture in Figure 7(b) can be used to identify the multi-featured plasmon responses of more complex
metallic nanostructures, such as nanoring, trimers and other nanoparticle aggregates. Intentionally,
dual or multiple resonant wavelength sensing can be achieved by nanodisk trimers [26], nanoring
trimers [27], and plasmonic oligomers [28]. Interaction of incident light with gold nanodisk trimers can
give rise to dual wavelength sensing. As the inter-gap distance among nanodisk trimers increases, dual
resonant peaks in visible and near infrared wavelength range are observed arising from the
electromagnetic coupling among the three disks.

Figure 7. (a) Various nanostructure designs based on the plasmon hybridization and
(b) simplified energy diagram for explaining the plasmon hybridization.

Moreover, Tao et al. reported that the sensitivity of nanoring trimers to the refractive index of the
surrounding medium is nearly three times larger than that of nanodisk trimers of comparable size [27].
Sensors 2011, 11 10916

This results from the plasmonic hybridization with a great tunability (ring size, wall thinkness and ring
separation). Due to complementary vibrational analysis of biomolecules combined with LSPR, the
enhancement of scattering light from such trimers can play a crucial role in the field of biological
sensing. Hence, multiple resonant wavelength sensing has originally developed from the complexed
nanostructures. This sensing method has been more distinguished for multiplexed bioassay. Tunable
plasmonic nanostructures consisting of periodic arrays of nanodisks and nanorings have also been
investigated theoretically and experimentally [2,29]. A nanoring, which is more complicated than a
nanodisk, can be fabricated by colloidal lithography and ion beam etching. When it is necessary to
have nano-scale small volumes for the detection of unlabeled, binding biomolecules, a nanoring may
confine the detection volume and be plugged in quantified biosensing applications. As shown in
Figure 8(a), a nanoring can confine induced electric fields into the nano-scale area as compared to a
nanodisk. Additional field enhancement can be achieved at the center of a nanoring due to the
plamonic hybridization. In designing the nanoring structure, nanoring width must be the critical
parameter. Figure 8(b) describes that narrower spectral linewidth at the visible-NIR spectrum can be
obtained as the nanoring width increases. Narrow spectral linewidth can be mentioned as high spectral
resolution. Spectral resolution at the nanoring might be determined by the nanoring width. It also
implies that this structure can have more degree of freedom than the nanodisk. However, the fabrication
of nanoring structure should be deliberately processed to make sure of a certain nanoring width.

Figure 8. (a) Induced electric field distributions (V/m) of nanodisk and nanoring structure,
respectively, at z = 25 nm. The outer radius and thickness of nanodisk and nanoring are
fixed at 50 nm, respectively. The width of nanoring is fixed at 30 nm. Incident electric field
is 1 (V/m). Surrounding medium is considered as an air (n = 1); (b) Spectrum of enhanced
amplitude with respect to the variation of inner radius at nanoring.

(a) (b)

Other representative nanostructures based on plasmonic hybridization are the nano-star [30] and
nano-pillar [31] structures. Hao et al. addressed the nanostar structure explicitly separating local
excitations [30]. A nanostar is composed of a central core from which a number of protruding tips
extend. They typically show an LSPR of the core and multiple LSPRs corresponding to the tips and core-
tip interactions. The latter are polarization dependent and accompanied by large local electric field
enhancements at the sharp ends of the tips. They revealed that several different plasmon modes can be
Sensors 2011, 11 10917

experimentally observed for a specific polarization state of the incident light. It is described by the
hybridization of plasmons associated with the core and individual tips of the nanoparticle. The electric
near-field enhancement arisen from tip plasmon modes is determined by the size of the core, as a result
of the hybridization of tip and core modes.
Individual plasmonic hot spots in a single gold nanostar can be selectively produced at the tips with
respect to the wavelength and polarization of incident light [32]. In order to investigate the optical
behavior of a nanostar in visible range, electric field distributions from a simplified nanostar structure
are numerically calculated in Figure 9. Unique property of three-dimensional structure can generate
specific field pattern with the variation of the polarization state. Resonant frequency or wavelength
is based on the length scale of individual tips assuming that core dimension is fixed. Due to the
complicated nano structures such as nanostar, a couple of plasmonic modes are generated. Each
plasmonic mode is closely correlated to the excited state of unit structure, corresponding to incident
polarization direction of light.

Figure 9. (a) Schematic of simplified nanostar placed onto a glass substrate. Electric field
distributions at a distance of 10 nm from a nanostar when illuminated by (b) horizontally
polarized light; (c) 45° polarized light; and (d) vertically polarized light.

3.3. Sensitivity Improvement Utilizing Fano Resonance and Electromagnetically Induced Transparency

Many researchers have paid attention to plasmonic structures that exhibit Fano resonances in their
optical spectra as a sensing platform. Fano resonance emerges from the coherent coupling and
interference of bright and dark plasmon modes [33]. A weak coupling and interference between a dark
and bright plasmon modes is fundamentally required for a Fano resonance. This coupling results from
symmetry breaking [34]. Another approach which can introduce a coupling between dark and bright
modes is launching an anisotropic environment, such as depositing a nanoparticle, or fabricating a
Sensors 2011, 11 10918

nanostructure by deposition methods, onto a dielectric substrate. This is mentioned as

substrate-induced Fano resonance as well. For a spherical nanoparticle in a vacuum, there is no
coupling between the bright dipolar and dark quadrupolar modes. However, when a nanoparticle is
placed onto the dielectric substrate, the image of a dipolar plasmon will obtain an established
quadrupolar field component across the nanoparticle, introducing a coupling between its dipolar and
quadrupolar plasmons. The resulting plasmon modes will be the superposition of both dipolar and
quadrupolar modes. They have appeared to be surprisingly more sensitive to the local dielectric
environment than the instinct plasmon modes of the nanostructure. In addition, electromagnetically
induced transparency (EIT) phenomenon can be manipulated by symmetry breaking. It is known as the
elimination of absorption via quantum interference in an atomic medium. Narrow transparency
resonance in the absorption spectrum is characterized by this phenomenon. This phenomenon would be
desirable for sensing applications due to narrow spectral resonant width. Liu et al. demonstrate that a
plasmonic EIT analogue can be achieved using a planar complementary metamaterial which consists
of cut-out structures in a homogeneous gold film [35].
3.4. Experimental Measurements of Various Nanostructures as LSPR Nanosensors

A variety of nanostructures have been experimentally exploited for the potential performance of LSPR
nanosensors recognizing the variation of local refractive index. The aforementioned nanostructures,
double nanocrescents and nanostar, are experimentally demonstrated [36,37]. Derived from single
nanocrescent, stacked double nanocrescents were implemented by colloidal lithography. The close
proximity of the nanocrescents leads to a new resonant coupling process. Additional multiple plasmonic
resonances are brought into double crescents. The plasmon hybridization picture can also be applied to
provide the physical description of double nanocrescents. Figure 10(a) shows that the overlapping of
double nanocrescents can create a dual resonant wavelength mode. The overlapping difference causes a
change in shift direction with respect to a single crescent resonance. The hybridization of nanocross and
nanobar (XI) can take to the coherent coupling of both bright and dark plasmon modes [38]. This
proposed structure might provide voluminous sensing areas by introducing a selective dry plasma etching
of the substrate which can be applied to a wide range of LSPR as well. When placed on a dielectric
substrate, the image of dipolar plasmon will bring into a significant quadrupolar field component across a
nanostructure, launching a coupling between dipolar and quadrupolar plasmons. The physical explanation
of this structure can also be supported by Fano resonance. Figure 10(b) shows the experimental results for
the 20 nm gap XI array. Three hybridized modes, characterized by the nanocross and nanobar, are
observed at extinction spectra. Multiwavelength spectroscopic sensing would be obtainable. The detailed
comparison of the bulk LSPR refractive index sensitivities was conducted. Different glycerol solutions
from 0% to 40% were supplied by a microfluidic chip. Triple hybridized modes lead to achievement of
high sensitivity up to 1,000 nm/RIU with this structure. Multiple resonance sensing can be observed at the
nanostars provided in Figure 10(c). Multiple LSPRs with respect to the tips and core-tip interactions are
monitored from scattering spectra. The longer wavelength resonances are polarization dependent. The tips
or the interaction between tips and core strongly influence on the longer wavelength resonances. Each
plasmonic mode is closely correlated to the excited state of unit structure, with respect to incident
polarization direction of light. Refractive index sensing was conducted by glucose water solutions with
refractive indexes ranging from 1 to 1.38. One of remarkable nanoparticle aggregates is plasmonic
Sensors 2011, 11 10919

oligomers, representing tailored optical properties [28]. Figure 10(d) shows the role of a center
nanoparticle in determining the resonant behavior of plasmonic oligomers. Fano resonance becomes more
dominant as the center particle diameter gets enlarged over 150 nm. A variety of array structures have
been experimentally verified as well. Periodic gold nanopillar system has been reported to introduce
complementary properties of localized and extended surface plasmons together [39]. This system is
characterized by monopole antenna arrays. Aligned gold nanotube arrays have been presented as
competitive refractive index sensors [40]. It claims that as the nanotube walls are exposed, the sensing
characteristic of inside and outside walls is differentiated.

Figure 10. Various nanostructures as the candidate of LSPR nano biosensor. (a)
Ultraviolet-visible-near-IR extinction spectra of stacked double crescents; (b) extinction
spectra and refractive index sensing results of XI cavity; (c) light scattering spectra of a
single gold nanostar and average spectral shift of nanostars resonances as a function of
surrounding refractive index; (d) extinction spectra of plasmonic octamers depending on
the center particle diameter for vertical and horizontal polarizations and (e) schematic of the
measurement system for LSPR sensing. Figures are reprinted with permission from [28,36-38].
(a) Copyright (2011) American Chemical Society (b) Copyright (2011) American
Chemical Society (c) Copyright (2010) American Chemical Society (d) Copyright (2011)
American Chemical Society.

(a) (b)
Sensors 2011, 11 10920

Figure 10. Cont.

Kabashin et al. introduced plasmonic nanorod metamaterials for biosensing [41]. They
demonstrated sensing improvement utilizing a plasmonic metamaterial that is subject to supporting an
anisotropic guided mode in a porous nanorod layer. By overlapping between the probing field and the
active biological substance, enhancement of sensitivity can be achieved after providing a strong
plasmon-mediated energy confinement. A typical measurement system for LSPR refractive index
sensing is based on a standard upright microscopy as shown in Figure 10(e). This setup can provide
spectral measurements from a broadband lamp and bright-field image capture by the use of CCD
camera. These notable nanostructures such as double nanocrescent, nanostar and plamsonic oligomers
are especially characterized by multiple resonant wavelengths. Multiple resonant modes can bring into
large spectral shift caused by the refractive index change.

4. Nano-Scale Applications of LSPR Sensors

4.1. Optical Antenna for Single Molecule Detection

Optical antennas analogous to microwave antennas have been viewed as the representative
nanostructure for single molecule detection. Optical fields can be confined to subdiffraction-limited
volumes and can be enhanced by the use of optical antennas [42-44]. The unique characteristics of
optical antennas allow detecting a few nano-scale molecule units. It is well known that the field
excitation and angular directivity of a nano-antenna can be controlled by the physical variables of the
antenna structure in analogy to microwave antennas. One of best nanostructures as an optical antenna
is a bowtie-shaped nanostructure [45]. Bowtie nanostructures are characterized by symmetrical sharp
tips, as compared to nanorods referred to as optical dipole antenna. Kinkhabwala et al. reported that gold
bowtie nano antenna shows the enhancement of single molecule's fluorescence up to a factor of 1,340,
ten times higher than previously experimented [46]. A single fluorescent molecule with transition
dipole behaves as a nanoscale optical sensor of the local electric field near a bowtie nanoantenna as
presented in Figure 11(a). Figure 11(b) presents a configuration for enhancing and controlling the
fluorescence emission of molecules diffusing in the central aperture reported by Aouani et al [47].
Fluorescent molecules are coupled to a single nanoaperture surrounded by periodic corrugations etched
in a thick gold film. The periodic circular corrugations act as a grating antenna reversibly coupling
light to surface plasmon wave.
Sensors 2011, 11 10921

Figure 11. Single molecule detection: (a) single-molecule fluorescence enhancements

produced by a bowtie nanoantenna; (b) unidirectional fluorescence emission of molecules
in a nanoaperture with plasmonic corrugations.

From this grating antenna, much higher transmission can be obtained through these corrugated
apertures than with standard noncorrugated apertures. In addition, they can achieve bright emission
and narrow directionality, which contribute to improving the detection of single molecules. Thus,
corrugated nanoapertures can provide a source for intense fluorescence light with narrow
directionality.
The optical Yagi-Uda antenna has been described as a fascinating nano-antenna, just like the radio
frequency (RF) Yagi-Uda antenna [48,49]. This nano-antenna can be applied to the technique of single
molecule detection due to directional far-field radiation. It is composed of an actively driven feed
element surrounded by a set of parasitic elements performing as reflectors and directors as shown in
Figure 12(a). Directional radiation from an optical Yagi-Uda antenna can be manipulated by the
number of directors and the length of reflector. Directors help emitting light from feed element to
propagate far more. Figure 12(b,c) indicate the angular directivity of an optical Yagi-Uda antenna with
the variation of the number of directors. It can be shown that the main lobe of the radiation pattern
becomes narrower and longer as the number of directors increases. Other important design parameters
for a Yagi-Uda antenna such as the lengths of the reflector and director are set to 1.05× (feed length)
and 0.9× (feed length), respectively. These values are chosen from [49], where they are optimized by
the design rules used in the microwave region.
Sensors 2011, 11 10922

Figure 12. (a) Schematic of optical Yagi-Uda antenna. Feed length of optical Yagi-Uda
antenna, wavelength of source, parameters ar, and ad are set to 160 nm, 570 nm, 130 nm,
and 143 nm, respectively. Polar radiation patterns with respect to the number n of directors
(b) at φ = 0° (y-z plane) and (c) φ = 90° (x-z plane).

4.2. Biological Applications with LSPR Nanosensors

The differences of local refractive index following biological interactions can be discerned utilizing
the exclusive properties of LSPR. Qualitative detection of biological interactions can be characterized
by employing organic molecules. Most organic molecules have a higher refractive index than buffer
solution. When organic molecules bind to nanoparticles, the local refractive index increases
accompanied with a red shift of the extinction spectrum. This mechanism makes possible the
recognition of biomolecules. Biomolecular recognitions have become imperative in clinical diagnostics
as well as in pharmacology [50,51]. In particular, LSPR acutely responds to the reactions occurring at
the surface of metallic nanostructures. LSPR nano-sensors can detect lipid membranes, protein binding
and up to DNA. A ligand-receptor interaction which appears on the plasma membrane can also be
probed with LSPR [4]. In an attempt to achieve fast, quantitative screening of ligand-receptor
interactions, lipid bilayers that resemble the native membrane environment must be probed by large
arrays of nanostructures illuminated by light. Thus, LSPR sensing technology is necessary to analyze
membrane proteins in native environments.
Sensors 2011, 11 10923

A supported lipid bilayer (SLB) is an in vitro system that mimics the plasma membrane in living
cells. SLB membranes can be made with a wide range of lipid compositions. They have sustained
lateral mobility that bears resemblance to a natural cell membrane. Label-free kinetic measurements of
biological membranes can be performed with a supported lipid bilayer. Real-time observations of the
formation and mobility of SLB membranes have been explored by SPR spectroscopy instead of
fluorescence tracking techniques [52]. Figure 13 illustrates lipid bilayers that are supported by
hydrophilic self-assembled monolayer (SAM) onto the gold nanostructure. SAM is necessary to mount
lipid membrane onto a noble metallic nanostructure. The difference in refractive index between a self
assembled monolayer and a lipid membrane can be optically detected with the noble metal
nanostructure. Membrane-bound proteins, which have a need of a lipid bilayer for intrinsic function,
can be monitored via LSPR sensing as seen in Figure 13. Membrane-mediated cytotoxicity of a
specific type of protein aggregates has attracted much interest due to its relation with conformational
diseases. Specifically, neurodegenerative diseases, including Alzheimer’s disease, Parkinson’s disease,
amyotrophic lateral sclerosis, Huntington’s disease, and Creutzfeldt–Jakob disease are caused by the
extracelluar and intracellular deposition of misfolded proteins in the form of aggregates of insoluble
amyloid [53]. Investigating the behavior of protein aggregates on a mimicking cell membrane is
regarded as a valuable approach to gain knowledge about cellular component-mediated cytotoxic
actions generated in vivo. These proteins act as the interface between a cell and its surroundings,
interposing responses to growth factors and immune cells.

Figure 13. Detection of supported lipid membrane and membrane-bound protein at the
gold nanostructure through LSPR peak shift.

Furthermore, protein binding events are specifically detected via LSPR nano-sensors [54,55]. One
of the typical proteins used for evaluating the performance of LSPR nano-sensors is biotin due to its
strong affinity with other conjugate proteins [2,37]. Biotin is defined as a water soluble B-complex
vitamin and is necessary for cell growth. Biotin strongly binds to avidin, streptavidin, and neutravidin
as biological receptor/ligand pairs. Before detecting specific protein binding events, bovine serum
albumin (BSA) is pre-used to eliminate non-specific binding interactions. Biotinylated bovine serum
albumin was absorbed onto the gold nanostructures. The glass surface was subsequently blocked for
protein binding by absorbing BSA before adding streptavidin solution. Figure 14 describes the sensing
of a binding event between biotin and streptavidin on a gold nanostructure. After streptavidin binds
with biotin, the resonant wavelength of the gold nanostructure is red-shifted. In an attempt to detect
wavelength shifts caused by protein binding more accurately, the LSPR nano-sensor should be
Sensors 2011, 11 10924

distinguished with the high spectral shift and narrow linewidth. In other examples of protein sensing,
attomole levels of the protein myoglobin on a SERS substrate were detected on a gold nanograin
aggregate array with interspacial distances down to 10 nm [12]. A highly reflective Al substrate
interacting with nanoparticles was able to detect refractive index changes of the specific interaction of
biomolecules including biotin and avidin, 5-fluorouracil and its antibody [56].

Figure 14. Detection of protein-protein binding event on the gold nanostructure through
LSPR peak shift.

DNA can be detected by the aforementioned sensing method, single molecule detection. It is beneficial
to detect a single molecule employing a few nanoscale structures such as nanodumbells [57]. These authors
report SERS-active gold-silver core-shell nanodumbbells where the gap between two nanoparticles,
Raman-dye position and environment can be engineered on the nanoscale. Single-DNA-tethered
nanodumbells can be utilized to detect Raman signals. Besides, a new sensing modality to detect the
target in a complex medium was proposed. Binding of target DNA takes to geometrical extension of
nanoparticle dimers [58]. It yields a spectral blue shift in the hybridized plasmon mode. In addition,
single-molecule detection of interleukin-2 by a silica microtoroid optical resonantor was demonstrated.
Single-molecule binding event leads to the shift of the resonant frequency [59].

5. Conclusions

In this paper, we have reviewed notable nanostructures for plasmonic sensing and explained relative
physical models. Optimized nanostructures exhibit not only intense field enhancement, but also high
spectral resolution. It is claimed that specific biological detection can be associated with definite
nanostructures. Table 1 presents the sorted characteristics of LSPR-based nanostructures. Diverse
nanostructures have been exploited for achieving optimal LSPR nanosensors. Appropriate
manipulation of geometrical parameters is a requirement for specific sensing purposes. However,
certain design limitations prevent further research for complete geometry of LSPR sensor. Remaining
challenges should be untangled, especially those concerning fabrication techniques and instrumental
resolution.
Sensors 2011, 11 10925

Table 1. Sensing characteristics of plasmonic nanostructures. ( RI : Refractive Index)

Wavelength Nanostructure Structure Dimensions Characteristic Sensitivity RI range Ref.

450–700 nm Silver spherical Diameter: 35 nm Shape-dependent LSPR 161 nm/RIU 1–1.6 [18]
nanoparticles

450–700 nm Silver triangular Diameter: 35 nm Shape-dependent LSPR 197 nm/RIU 1–1.6 [18]
nanoparticles

450–700 nm Silver rodlike Aspect ratio 5:1 Shape-dependent LSPR 235 nm/RIU 1–1.6 [18]
nanoparticles Diameter: 35nm

800–1,000 nm Gold nano rods Aspect ratio 3.5:1 Size-dependent LSPR 650 nm/RIU 1.34–1.7 [60]
Radius: 40 nm

450–600 nm Gold colloidal Diameter: 30 nm Shape-dependent LSPR 70.9 nm/RIU 1.32–1.5 [61]
nanoparticles

400–800 nm Hollow gold Diameter: 50 nm Shape-dependent LSPR 408 nm/RIU 1.32–1.5 [61]
nano shell Wall thickness: 4.5 nm

500–1,000 nm Arrays of gold Pitch of nanodisk: Anisotropic property 167 nm/RIU 1.32–1.42 [29]
nanodisk 162 nm, 340 nm of gold nanodisk 327 nm/RIU

600–750 nm Gold nanodisk Small disk diameter: 96 nm Visible and near- 170 nm/RIU 1–1.5 [26]
1,100–1,400 trimers Larger disk diameter: 127 nm infrared localized 373.9nm/RIU
nm Pitch between trimers: 400 nm surface plasmon
resonances

900–1,500 nm Gold nanorings Diameter: 150 nm Shape dependence 880 nm/RIU 1.33–1.42 [2]
Thickness: 20 nm on dielectric substrate

500–1,700 nm Gold nanoring Outer diameter:120 nm Plasmon hybridization 345 nm/RIU 1–1.5 [27]
trimers Wall thickness: 33 nm
Ring height: 24 nm

350–650 nm Nanocubes Size : 100 nm Sharp quadripolar 165 nm/RIU Neutravidin [4]
LSPR peak binding

800–2,800 nm Nanocrescents Diameter: 410 nm Plasmon-induced 879 nm/RIU Streptavidin [3]

Deposition angle:10° electromagnetic near- binding
Aspect ratio: 4 field

550–750 nm Nanostars Core size: 30–50 nm Multiple plasmon 218 nm/RIU 1–1.38 [37]
Conical tips: 10–60 nm Resonances

1200–1,900 Nanocross and Length: 380nm Subradiant 710 nm/RIU 1.333–1.38 [38]
nm nanobar Width: 76 nm Fano resonances 1,000
α = 60° nm/RIU

1,361 nm Double nanopillars Diameter: 425 nm Plasmon electromagnetic 642 nm/RIU 1.34–1.44 [31]
1,512 nm with nanogap Height: 288 nm field induced by nanogap 1,056
Nanogap: 33 nm nm/RIU
Sensors 2011, 11 10926

Table 1. Cont.

Wavelength Nanostructure Structure Dimension Characteristic Sensitivity RI range Ref.

950–2,500 nm Planar Length: 400 nm, 340 nm Electromagnetically 725 nm/RIU 1.332–1.372 [35]
metamaterials Width: 80 nm, 90 nm induced transparency
analogue of EIT Gap: 45 nm

400–1,000 nm Plasmonic nanorod Length: 20–700 nm Anisotropic guided 30,000 nm/RIU 1–1.36 [41]
metamaterials Diameter: 10–50 nm mode
Pitch: 40–70 nm

550–900 nm Arrays of Length: 120 nm Shape-dependent 250 nm/RIU 1.333–1.368 [40]

plasmonic Inner diameter: 22 nm LSPR
nanotubes Outer diamete: 44 nm
Pitch: 55 nm

750–1,000 nm Nanopillar arrays Radius: 100 nm Monopole antenna 675 nm/RIU 1.33–1.45 [39]
Height: 400 nm arrays
Pitch: 600 nm

Acknowledgments

This work was supported by the National Research Foundation and the Ministry of Education,
Science and Technology of Korea through the Creative Research Initiatives Program (Active
Plasmonics Application Systems).

References

1. Tan, Y.N.; Su, X.; Zhu, Y.; Lee, J.Y. Sensing of transcription factor through controlled-assembly
of metal nanoparticles modified with segmented DNA elements. ACS Nano 2010, 4, 5101-5110
2. Larsson, E.M.; Alegret, J.; Kall, M.; Sutherland, D.S. Sensing characteristics of NIR localized
surface plasmon resonances in gold nanorings for application as ultrasensitive biosensors. Nano
Lett. 2007, 5, 1256-1263.
3. Bukasov, R.; Ali, T.A.; Nordlander, P.; Shumaker-Parry, J.S. Probing the plasmonic near-field of
gold nanocrescent antennas. ACS Nano 2010, 4, 6639-6650.
4. Galush, W.J.; Shelby, S.A.; Mulvihill, M.J.; Tao, A.; Yang, P.; Groves, J.T. A nanocube
plasmonic sensor for molecular binding on membrane surfaces. Nano Lett. 2009, 9, 2077-2082.
5. Kim, D.K.; Park, T.J.; Tamiya, E.; Lee, S.Y. Label-free detection of leptin antibody-antigen
interaction by using LSPR -based optical biosensor. J. Nanosci. Nanotechnol. 2011, 11, 4188-4193.
6. Stewart, M.E.; Anderton, C.R.; Thompson, L.B.; Maria, J.; Gray, S.K.; Rogers, J.A.; Nuzzo, R.G.
Nanostructured plasmonic sensors. Chem. Rev. 2008, 108, 494-521.
7. Lee, B.; Roh, S.; Park, J. Current status of micro-and nano-structured optical fiber sensors. Opt.
Fiber Technol. 2009, 15, 209-221.
8. Svedendahl, M.; Chen, S.; Dmitriev, A.; Kall, M. Refractometric sensing using propagating
versus localized surface plasmons. Nano Lett. 2009, 9, 4428-4433.
Sensors 2011, 11 10927

9. Anker, J.N.; Hall, W.P.; Lyandres, O.; Shah, N.C.; Zhao, J.; Van Duyne, R.P. Biosensing with
plasmonic nanosensors. Nat. Mater. 2008, 7, 442-453.
10. Jain, P.K.; El-Sayed, M.A. Plasmonic coupling in noble metal nanostructures. Chem. Phys. Lett.
2010, 487, 153-164.
11. Oh, Y.-J.; Park, S.-G.; Kang, M.-H.; Choi, J.-H.; Nam, Y.; Jeong, K.-H. Beyond the SERS:
Raman enhancement of small molecules using nanofluidic channels with localized surface
plasmon resonance. Small 2011, 7, 184-188.
12. Das, G.; Mecarini, F.; Angelis, F.D.; Prasciolu, M.; Liberale, C.; Patrini, M.; Fabrizio, E.D.
Attomole myoglobin Raman detection from plasmonic nanostructures. Microelectron. Eng. 2008,
85, 1282-1285.
13. Homola, J. Electromagnetic Theory of Surface Plasmons. In Surface Plasmon Resonance Based
Sensors; Springer: Berlin, Germany, 2006; Volume 4, pp. 3-44.
14. Liedberg, B.; Nylander, C.; Lunstrom, I. Surface plasmon resonance for gas detection and
biosensing. Sens. Actuat. 1983, 4, 299-304.
15. Liao, P.F.; Wokaun, A. Lightning rod effect in surface enhanced Raman scattering. J. Chem.
Phys. 1982, 76, 751-752.
16. Zhu, J.; Li, F.-K. Effect of aspect ratio on the inter-surface plasmonic coupling of tubular gold
nanoparticle. Eur. Phys. J. B 2011, 80, 83-87.
17. Jain, P.K.; El-Sayed, M.A. Noble metal nanoparticle pairs: Effect of medium for enhanced
nanosensing. Nano Lett. 2008, 8, 4347-4352.
18. McFarland, A.D.; Van Duyne, R.P. Single silver nanoparicles as real-time optical sensors with
zeptomole sensitivity. Nano Lett. 2003, 3, 1057-1062.
19. Kim, H.M.; Jin, S.M.; Lee, S.K.; Kim, M.; Shin, Y. Detection of biomolecular binding through
enhancement of localized surface plasmon resonance (LSPR) by gold nanoparticles. Sensors
2009, 9, 2334-2344.
20. Wiley, B.J.; Chen, Y.; McLellan, J.M.; Xiong, Y.; Li, Z.-Y.; Ginger, D.; Xia, Y. Synthesis and
optical properties of silver nanobars and nanorice. Nano Lett. 2007, 7, 1032-1036.
21. Wei, H.; Reyes-Coronado, A.; Nordlander, P.; Aizpurua, J.; Xu, H. Multipolar plasmon
resonances in individual Ag Nanorice. ACS Nano 2010, 4, 2649-2654.
22. Hanarp, P.; Kall, M.; Sutherland, D.S. Optical properties of short range ordered arrays
of nanometer gold disks prepared by colloidal lithography. J. Phys. Chem. B 2003, 107, 5768-5772.
23. Wu, L.Y.; Ross, B.M.; Lee, L.P. Optical properties of the crescent-shaped nanohole antenna.
Nano Lett. 2009, 9, 1956-1961.
24. Prodan, E.; Radloff, C.; Halas, N.J.; Nordlander, P. A hybridization model for the plasmon
response of complex nanostructures. Science 2003, 302, 419-422.
25. Lassiter, J.B.; Azipurua, J.; Hernandez, L.I.; Brandl, D.W.; Romero, I.; Lai, S.; Hafner, J.H.;
Nordlander, P.; Halas, N.J. Close encounters between two nanoshells. Nano Lett. 2008, 8, 1212-1218.
26. Tripathy, S.; Mlayah, A. Dual wavelength sensing based on interacting gold nanodisk trimers.
Nanotechnology 2010, 21, 305501.
27. Lin, V.K.; Teo, S.L.; Marty, R.; Arbouet, A.; Girard, C.; Alarcon-Llado, E.; Liu, S.H.; Han, M.Y.;
Teo, S.L.; Lin, V.K.; Gold nanoring trimers: A versatile structure for infrared sensing. Opt.
Express 2010, 18, 22271-22282.
Sensors 2011, 11 10928

28. Hentsch, M.; Dregely, D.; Vogelgesang, R.; Giessen, H.; Liu, N. Plasmonic oligomers: The role
of individual particles in collective behavior. ACS Nano 2011, 5, 2042-2050.
29. Lee, S.-W.; Lee, K.-S.; Ahn, J.; Lee, J.-J.; Kim, M.-G.; Shin, Y.-B. Highly sensitive biosensing
using arrays of plasmonic Au nanodisks realized by nanoimprint lithography. ACS Nano 2011, 5,
897-904.
30. Hao, F.; Nehl, C.L.; Hafner, J.H.; Nordlander, P. Plasmon resonances of a gold nanostar. Nano
Lett. 2007, 7, 729-732.
31. Kubo, W.; Fujikawa, S. Au double nanopillars with nanogap for plasmonic sensor. Nano Lett.
2011, 11, 8-15.
32. Hrelescu, C.; Sau, T.K.; Rogach, A.L; Jackel, F.; Laurent, G.; Douillard, L.; Charra, F. Selective
excitation of individual plasmonic hotspots at the tips of single gold nanostars. Nano Lett. 2011,
11, 402-407.
33. Zhang, S.; Bao, K.; Halas, N.J.; Xu, H.; Nordlander, P. Substrate-induced Fano resonances of a
plasmonic nanocube: A route to increased-sensitivity localized surface plasmon resonance sensors
revealed. Nano Lett. 2011, 11, 1657-1663.
34. Gomez, D.E.; Vernon, K.C.; Davis, T.J. Symmetry effects on the optical coupling between
plasmonic nanoparticles with applications to hierarchical structures. Phys. Rev. B 2010, 81, 075414.
35. Liu, N.; Weiss, T.; Mesch, M.; Langguth, L.; Eigenthaler, U.; Hirscher, M.; Sonnichsen, C.;
Giessen, H. Planar metamaterial analogue of electromagnetically induced transparency for
plasmonic sensing. Nano Lett. 2010, 10, 1103-1107.
36. Vogel, N.; Fischer, J.; Mohammadi, R.; Retsch, M.; Butt, H.-J.; Landfester, K.; Weiss, C.K.;
Kreiter, M. Plasmon hybridization in stacked double crescents arrays fabricated by colloidal
lithography. Nano Lett. 2011, 11, 446-454.
37. Dondapati, S.K.; Sau, T.K.; Hrelescu, C.; Klar, T.A.; Stefani, F.D.; Feldmann, J. Label-free
biosensing based on single gold nanostars as plasmonic transducers. ACS Nano 2010, 4, 6318-6322.
38. Verellen, N.; Dorpe, P.V.; Huang, C.; Lodewijks, K.; Vandenbosch, G.A.E.; Lagae, L.;
Moshchalkov, V.V. Plasmon line shaping using nanocrosses for high sensitivity localized surface
Plasmon resonance sensing. Nano Lett. 2011, 11, 391-397.
39. Cetin, A.E.; Yanik, A.A.; Yilmaz, C.; Somu, S.; Busnaina, A.; Altug, H. Monopole antenna arrays
for optical trapping, spectroscopy, and sensing. Appl. Phys. Lett. 2011, 98, 111110.
40. McPhillips, J.; Murphy, A.; Jonsson, M.P.; Hendren, W.R.; Atkinson, R.; Hook, F.; Zayats, A.V.;
Pollard, R.J. High-performance biosensing using arrays of plasmonic nanotubes. ACS Nano 2010,
4, 2210-2216.
41. Kabashin, A.V.; Evans, P.; Pastkovsky, S.; Hendren, W.; Wurtz, G.A.; Atkinson, R.; Pollard, R.;
Podolskiy, V.A.; Zayats, A.V. Plasmonic nanorod metamaterials for biosensing. Nat. Mater. 2009,
8, 867-871.
42. Greffet, J.-J. Nanoantennas for light emission. Science 2005, 308, 1561-1563.
43. Park, Q.-H. Optical antennas and plasmonics. Contemp. Phys. 2009, 50, 407-423.
44. Pakizeh, T.; Kall, M. Unidirectional ultracompact optical nanoantennas. Nano Lett. 2009, 9,
2343-2349.
45. Yu, N.; Cubukcu, E.; Diehl, L.; Bour, D.; Corzine, S.; Zhu, J.; Hofler, G.; Crozier, K.B;
Capasso, F. Bowtie plasmonic quantum cascade laser antenna. Opt. Express 2007, 15, 13272-13281.
Sensors 2011, 11 10929

46. Kinkhabwala, A.; Zongfu, Y.; Fan, S.; Avlasevich, Y.; Mullen, K.; Moerner, W.E. Large
single-molecule fluorescence enhancements produced by a bowtie nanoantenna. Nat. Photonics
2009, 3, 654.
47. Aouani, H.; Mahboub, O.; Bonod, N.; Devaux, E.; Popov, E.; Rigneault, H.; Ebbesen, T.W.;
Wenger, J. Bright unidirectional fluorescence emission of molecules in a nanoaperture with
plasmonic corrugations. Nano Lett. 2011, 11, 637-644.
48. Kosako, T.; Kadoya, Y.; Hofmann, H.F. Directional control of light by a nano-optical Yagi-Uda
antenna. Nat. Photonics 2010, 4, 312-315.
49. Taminiau, T.H.; Stefani, F.D.; Van Hulst, N.F. Enhanced directional excitation and emission of
single emitters by a nano-optical Yagi-Uda antenna. Opt. Express 2008, 16, 10858-10866.
50. Wang, Y.; Qian, W.; Tan, Y.; Ding, S. A label-free biosensor based on gold nanoshell monolayers
for monitoring biomolecular interactions in diluted whole blood. Biosens. Bioelectron. 2008, 23,
1166-1170.
51. Marinakos, S.; Chen, S.; Chilkoti, A. Plasmonic detection of a model analyte in serum by a gold
nanorod sensor. Anal.Chem. 2007, 79, 5278-5283.
52. Maynard, J.A.; Lindquist, N.C.; Sutherland, J.N.; Lesuffleur, A.; Warrington, A.E.;
Rodriguez, M.; Oh, S.-H. Surface plasmon resonance for high-throught ligand screening of
membrane-bound proteins. Biotechnol. J. 2009, 4, 1542-1558.
53. Krazinski, B.E.; Radecki, J.; Radecka, H. Surface plasmon resonance based biosensors for exploring
the influence of alkaloids on aggregation of amyloid-β Peptide. Sensors 2011, 11, 4030-4042.
54. Raschke, G.; Kowarik, S.; Sonnichsen, F.C.; Klar, T.A.; Feldmann, J.; Nichtl, A; Kurzinger, K.
Biomolecular recognition based on single gold nanoparticle light scattering. Nano Lett. 2003, 3,
935-938.
55. Xu, J.; Zhang, L.; Gong, H.; Homola, J.; Yu, Q. Tailoring plasmonic nanostructures for optimal
SERS sensing of small molecules and large microorganisms. Small 2011, 7, 371-376.
56. Hiep, H.M.; Yoshikawa, H.; Tamiya, E. Interference localized surface plasmon resonance
nanosensor tailored for the detection of specific biomolecular interactions Anal. Chem. 2010, 82,
1221-1227.
57. Lim, D.K.; Jeon, K.-S.; Kim, H.-M.; Nam, J.-M.; Suh, Y.D. Nanogap-engineerable Raman-active
nanodumbbells for single-molecule detection. Nat. Mater. 2010, 9, 60-67.
58. Chen, J.I.L.; Chen, Y.; Ginger, D.S. Plasmonic nanoparitlce dimers for optical sensing of DNA in
complex media. J. Am. Chem. Soc. 2010, 132, 9600-9601.
59. Armani, A.M.; Kulkarni, R.P.; Fraser, S.E.; Flagan, R.C.; Vahala, K.J. Label-free, single molecule
detection with optical microcavities. Science 2007, 317, 783-787.
60. Lee, K.-S.; El-Sayed, M.A. Gold and silver nanoparticles in sensing and imaging. J. Phys. Chem. B
2006, 110, 19220-19225.
61. Sun, Y.; Xia, Y. Increased sensitivity of surface plasmon resonance of gold nanoshells compared to
that of gold solid colloids in response to environmental changes. Anal. Chem. 2002, 74, 5297-5305.

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