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Plasmonics

https://doi.org/10.1007/s11468-023-02154-8

RESEARCH

Metallic Nanodisk‑in‑Elliptical Nanohole Array Based Fiber Tip


for Enhanced Plasmonic Refractometric Sensing
Zhenshi Chen1 · Xincheng Huang1 · Hui Zhang2

Received: 30 October 2023 / Accepted: 30 November 2023


© The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature 2023

Abstract
In this work, a high performance surface plasmon resonance (SPR) fiber sensor based on metallic elliptical nanohole and
circular nanodisk binary array has been theoretically designed and investigated. The binary array structure is integrated on
the end facet of optical fiber to excite SPR and generate three optical resonance dips in reflection spectra in the near-infrared
region. The first resonance dip not only fits the characteristics of narrow linewidth, but also has the advantages of high peak-
to-dip signal ratio and sensitivity. When the external environment changes in the refractive index (RI) range of 1.33 ~ 1.40, a
high RI sensitivity of 669 nm/RIU, a narrow FWHM of 5.8 nm, and a high FOM value of 115.3 are yielded simultaneously
for the first dip. Compared to unitary nanostructure arrays, the composite plasmonic structure of nanodisk and elliptical
nanohole array demonstrated here can generate SPR modes with sharper spectral feature which is crucial to high sensitivity
and precision detection technology. These features make our proposed plasmonic fiber tip sensor highly promising in terms
of high-performance biosensing applications.

Keywords Surface plasmon resonance · Lab on fiber · Fiber sensor · Plasmonic nanostructure

Introduction and label-free plasmonic biosensors as a promising and valid


alternative to conventional diagnostic tools can contribute
Surface plasmon resonance (SPR) supported by metallic to rapid and massive diagnostics for infectious diseases [4].
nanostructures can generate highly enhanced local elec- Furthermore, with advances in nanophotonics and nanofab-
tromagnetic fields strongly depend on the surrounding rication technology, “Lab on fiber” (LOF) technologies can
environments, which create a new route for designing high- transfer functionalized plasmonic nanostructure onto the
sensitivity biosensors. Due to their distinctive capacity in fiber end facet, so as to fulfil the fiber tip SPR sensors for
rapid label-free detection of biochemical substances, SPR miniature size, lightweight, easy-to-use, low cost and remote
sensors have the potential to become an important tool in sensing [5]. This makes them very attractive for the design
molecular biology and medical diagnostics. Traditional of portable devices for point-of-care testing (POCT) applica-
diagnostic techniques essentially rely on polymerase chain tion. The development of advanced optical fiber tip sensing
reaction (PCR) tests [1], which need relatively long time probe is expected to directly carry out real-time and in vivo
to identify diagnostic results, thus delay massive detection. diagnosis and biomedical detection.
Nanoplasmonic biosensors based on SPR nanostructure The plasmonic periodic nanostructures, commonly
array have been reported for direct detection of live viruses formed by patterned metallic nanostructure arrays, can sup-
and cells from biological media in real time [2, 3]. The fast port propagating surface plasmons (PSP) mode and highly
field-enhanced localized surface plasmon resonance (LSPR)
mode which largely depends on the shape and size of the
* Xincheng Huang
huangxincheng@zjhzu.edu.cn metallic nanostructures [6]. Different plasmonic nanostruc-
ture shapes including triangular gold nanopillars [7], Au
1
School of Electronic Information, Huzhou College, elliptical nanoholes [8], square Au nanopatches or nano-
Huzhou 313000, China holes [9], and circular nanodisks [10] have been employed in
2
School of Physics and Optoelectronic Engineering, sensing applications. These plasmonic nanostructure sensors
Guangdong University of Technology, Guangzhou 510006, show rapid and highly sensitive detection; however, they
China

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Plasmonics

usually have a great limitation: the resonance modes of the the narrow linewidth and high RI sensitivity enables dip
plasmonic nanoarray, especially LSPR modes, are always A produce a high figure of merit (FOM) value of 115.3,
accompanied by a relatively wide spectral feature with low which is more than 7.1 times larger compared to that of
resonance dip contrast ratio because of strong radiative unitary nanohole arrays. Moreover, the binary array-based
damping which heavily limits their sensing performance. plasmonic structures exhibit strong polarization-dependent
Hence, how to suppress the radiative damping is an essential reflection spectrum characteristics. The proposed fiber SPR
question in the plasmonic sensing field. Up to now, some sensing structure is promising for developing high perfor-
groping strategies are adopted to reduce radiation damping, mance biosensors and optical polarizing devices and thereby
such as, asymmetric Fano-type resonance [11], and subradi- boost their potential applications in biological detection and
ant plasmon mode excitation [12]. In this work, a circular medical diagnosis fields.
nanodisk-in-elliptical nanohole binary array (CNENBA)
supporting different SPR modes with resonantly enhanced
coupling interaction is theoretically proposed to suppress the Structure Design and Numerical Simulations
radiative damping, and thereby to achieve narrow spectral
width and improved plasmonic sensing performance. This To improve the sensing performance of an RI sensor, it is
CNENBA-based plasmonic nanostructure integrated on the essential to excite a resonance spectrum with narrow spectral
end facet of optical fiber generates three SPR resonance dips width and large peak or dip contrast ratio, which is possible
(marked by A, B, and C) in reflection spectra in the near- to be achieved by exciting the coupled resonance plasmonic
infrared wavelength region. Here, the resonance dip A, as a modes in an elaborate binary metallic nanostructure array.
top surface resonance mode, not only fits the characteristics Integrating functionalized plasmonic nanostructure
of narrow spectral width, but also has the advantages of high onto the fiber end facet can fulfil the fiber-tip SPR sen-
peak-to-dip signal ratio and large sensitivity to the changes sors that are miniature-sized, lightweight, easy-to-use, and
of sensing medium. When the external environment alters in suitable for remote sensing. Figure 1 depicts the structure
the refractive index (RI) range of 1.33 ~ 1.40, a high RI sen- schematic diagram of the proposed CNENBA-based fiber
sitivity of 669 nm/RIU, and a much sharper spectral feature, tip sensor. As shown in Fig. 1, the CNENBA structure
as narrow as 5.8 nm of full width at half maximum (FWHM) is constructed by spatially embedding concentric circular
are obtained for the resonance dip A. The combination of nanodisks into elliptical nanoholes. The gap between the

Fig. 1  a Schematic of the Px


plasmonic fiber tip sensor with
CNENBA integrated on the (a) (b)
fiber end facet. b The magnified
view for a 3×3 nanostructure
array with structural param-
eters marked. c The reflection d
spectrum of CNENBA structure
at ambient RI of 1.33 D2
D1
Py

y
x
(c)

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Plasmonics

elliptical hole and circular disk forms an irregular nanor- Numerical Results and Discussion
ing which supports different SPR modes excitation and
coupling interaction. This CNENBA nanostructure can Plasmonic Resonance Mode Analysis
be fabricated onto the fiber end facet by conventional
nanofabrication methods, such as electron-beam lithog- To understand the inherent physical mechanism of these res-
raphy (EBL) [10], focused-ion beam (FIB) milling [13] onance dips in detail, we calculated and analyzed the mode
or template transfer method [14] and so on. The fiber tip field profiles for the CNENBA-based SPR structure at the
SPR sensor integrated with CNENBA-based plasmonic resonance wavelengths. Three pairs of monitor slices are set
nanostructure on the end facet generates three plasmonic at a plane 2 nm away from the top (or bottom) surface of the
resonance dips (marked by A, B, and C) in reflection spec- CNENBA gold film and the cross section of two unit cells
tra in the near-infrared wavelength region. in x–z plane to record the distributions of the most dominant
The numerical calculations are performed with finite- electric field component Ez for dips A, B, and C, which are
difference time domain (FDTD) method (implemented in a presented in Fig. 2a–f respectively.
full-wave simulation software, Lumerical FDTD solutions) By observing Fig. 2a, b, it can be clearly found that apart
to obtain the reflection spectra and electric field distribution from the coexisted LSPR mode around the annular aperture,
of the CNENBA structure. In the simulation, an x-polarized the electric field distribution for dip A (at resonant wave-
plane light source with electric field amplitude of 1 V/m length 920 nm) is mainly concentrated at the metal/ambient
perpendicularly illuminates on the CNENBA structure from medium interface, which has a long exponential decay depth
the high RI fiber side. Periodic boundary conditions are into the medium side and exhibits the distinct PSP mode
applied in X and Y directions, while perfectly matched lay- characteristics [15]. This top surface mode extending deep
ers are used in Z direction. Fine meshes with dx = dy = 1 nm into the surrounding medium greatly enhances the interac-
and dz = 2 nm are used in the narrowest structural region, tion volume between the ambient medium and optical field,
and combination of grading mesh and conformal meshing which can offer larger sensitivity to the RI variation of the
method offered by the software package is implemented to sensing medium. The resonance mode for dip B (at resonant
ensure the accurate convergence of the numerical results. wavelength 1003 nm) behaves similarly to dip A, as illus-
The surrounding of the fiber-tip plasmonic structure is trated in Fig. 2c, d. The difference is that the electric field for
covered with a sensing medium with RI of 1.33, achieving dip B is excited as a SPR mode at the bottom surface of gold
the matching effect of the aqueous analyte in the practi- film and mainly confined at the metal/fiber interface, which
cal detection. Figure 1c exhibits the calculated reflection exponentially decays into the high RI fiber substrate side.
spectrum, corresponding to the optimized structure param- For this reason, dip B is insensitive to the external environ-
eters as follows: periods Px = 680 nm and Py = 620 nm, disk ment RI variation. In contrast, the electric field distribution
diameter d = 90 nm, elliptical nanohole long axis diameter for dip C (at resonant wavelength 1161 nm) represents a
D1 = 240 nm, short axis diameter D 2 = 120 nm, and the typical LSPR mode, as illustrated in Fig. 2e, f. Due to much
thickness of Au film H = 80 nm. The geometric parameters larger radiation damping for LSPR mode compared with that
are depicted in Fig. 1b. In the simulation, the light is set to of strongly coupled SPR modes, the resonance dip C has
radiate from the core of the fiber, passes through the nano- much broader linewidth of reflection spectrum than that of
structure where it is partly absorbed, and then reflects back dips A and B, where the strong coupling interaction of coex-
to the core of the fiber. Through analyzing the reflected isted PSP and LSP modes leads to the resonantly enhanced
spectrum of light received from fiber end, three resonance optical transmission and absorption with sharp spectral fea-
dips with high peak-to-dip signal ratio can be observed at ture, as shown in the reflection spectrum in Fig. 1c.
923 nm, 1002 nm, and 1161 nm indicated by red symbol A,
B, and C respectively, as displayed in Fig. 1c. These three Geometrical Parameter Effect
resonance dips stem from different SPR modes excitation
and coupling interaction that lead to resonantly enhanced For further understanding the optical properties of the
optical transmission and absorption at different resonant proposed CNENBA structure, we calculated and observed
frequency positions. It also can be found in Fig. 1c that the the evolution of SPR reflection spectra with the changes
spectral linewidths of dips A and B are much narrower than of geometrical parameters, as depicted in Fig. 3. Here,
that of dip C (5.8 nm and 11.4 nm vs 124.7 nm). Moreover, the structure parameters, the period in X direction (Px),
their sharpness is superior to those ever reported plasmonic CNENBA gold film thickness (H), and the short axis diam-
nanostructures [7, 8, 10]. These narrow spectral features of eter (D2) of the elliptical nanohole, are mainly focused on
resonance dips play crucial roles on improving the sensing for investigating their impacts on the optical spectrum
performance for biosensing applications. response. Figure 3a illustrates the role of thickness (H)

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Plasmonics

Fig. 2  The z component of electric field E


­ z distributions located at 2 nm distance from the bottom surface of gold film for dip B; b, d, f
different sections in the CNENA system: a, e at 2-nm distance from through the center of binary structure along x–z plane for dips A, B,
the top surface of gold film for dips A and C, respectively; c at the and C

played in the reflection spectra evolution. Clearly, increas- a slight trend towards narrower spectral linewidths. This
ing the thickness of gold film (H > 100 nm) would result is because with the increase of thickness H, the LSPR
in a shallower depth for resonance dips A and B. This is mode gradually converts to the cavity mode in annular
primarily due to the decoupling of the coexisting resonance aperture well, which mainly localizes in the cavity well
modes at top and bottom surfaces of gold film, which with reduced radiation loss. The resonance dip sharpness
reduces the dissipation within the film. However, for dips is mainly determined by the spectral linewidth and peak-to-
A and B, if the gold film is too thin (H < 50 nm), the dis- dip signal ratio. In order to ensure the narrow FWHM and
sipation of SPR modes in the gold film will be reduced due large contrast ratio of dips A and B, the thickness of gold
to the weakened localization of SPR modes. In the case film (i.e., H = 80 nm) was chosen as optimal plasmonic
of dip C, as the thickness of gold film increases, there is film thickness for further analysis.

Fig. 3  The reflection spectra


evolution with a gold film
thickness increasing from 50 to
170 nm, b period along X direc-
tion Px increasing from 620 to
740 nm, c short axis diameter
D2 of the elliptical hole increas-
ing from 120 to 240 nm. When
one parameter is surveyed,
other unconcerned parameters
are fixed: gold film thick-
ness H = 80 nm, array periods
Px = 680 nm and Py = 620 nm,
nanodisk diameter d = 90 nm,
long axis diameter of elliptical
nanohole D1 = 240 nm and its
short axis diameter D2 = 120 nm

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Plasmonics

The effect of period in X direction Px on the three reso- the elliptical hole is set as 120 nm in the designed structure.
nance dips is shown in Fig. 3b. With the increase of binary From the above analysis and comparison, the finally opti-
array period Px, the resonance wavelengths of dips A and mized geometrical parameters of the design structure are
B exhibit more remarkable red shift than that of dip C, as obtained as below: the gold film thickness H = 80 nm, the
illustrated in Fig. 3b. This provides further evidence that dip array periods Px = 680 nm and Py = 620 nm, the nanodisk
C is associated with the dominant LSPR mode, whereas dips diameter d = 90 nm, the long axis diameter of elliptical nano-
A and B are relevant to the dominant PSP modes, which are hole D1 = 240 nm and its short axis diameter D2 = 120 nm.
excited in the binary array by grating effect closely depend- Herein, it needs to point out that narrower spectral linewidth
ing on the structure period Px. The period in Y direction for both dips A and B can be obtained by increasing the
Py hardly exerts influence on the resonance wavelengths of nanodisk diameter d. However, considering the feasibility of
dips A and B (its corresponding reflection spectrum evo- the actual fabrication, the diameter d is fixed at a moderate
lution is not provided in the figure), evidencing a polari- value of 90 nm in the structural optimization.
zation dependence of this structure. The structural periods
Px = 680 nm and Py = 620 nm are selected for the sharper
RI Sensing Performance
spectral feature after taking a comparative analysis in
Fig. 3b. For the theoretical analysis of this rectangle period
To assess the sensing performance of the proposed SPR
lattice, the resonance modes at the metal/dielectric interface
sensor based on CNENBA and compare it with other
can be given by Bragg’s coupling equation [16]:
reported nanostructures, we quantitatively investigate
2𝜋 2𝜋

𝜀 m 𝜀d and discuss two major parameters: bulk sensitivity (S)
���
⃗ ��

sin 𝜑 ± iGx ± jGy = (1)
𝜆res 𝜆res 𝜀m + 𝜀d and FOM. Figure 4a provides the reflection spectrum
evolution for the design with the different surrounding
where εm and εd are the dielectric constants of metal and sur- environmental RIs in the range of 1.33–1.40. It can be
rounding medium respectively, λres and φ are the respective obviously seen that the reflection spectra of the two SPR
resonance dip wavelength and incident angle, and Gx = 2π/Px modes (dips A and B) maintain narrow FWHM and high
and Gy = 2π/Py, are reciprocal lattice constant along the x- contrast ratio in the wide RI range. Comparatively, the
and y-axis respectively. The i and j are integer multiples, dip C possesses broad FWHM in the whole RI range.
which correspond to the (i, j) diffraction order associated Moreover, three resonant dips A, B and C exhibit red
with the light transmission through the periodic nanohole shift with different magnitude when the RI increases
array. For normal incidence of x-polarized light, φ is 0. from 1.33 to 1.40. The difference of resonance wave-
According to Eq. (1), the resonance wavelengths for dips length shift amount means different RI sensitivities. For
A and B are calculated to be 929 nm and 1012 nm, respec- describing the sensing sensitivities more intuitively, the
tively. These theoretically calculated wavelength values resonant wavelengths are plotted as the functions of sens-
are both in good agreement with the numerical simulation ing RI for dips A, B, and C in Fig. 4b. Linear fittings
results in Fig. 1, confirming that dips A and B arise from the are implemented to indicate the change trend of the reso-
(1, 0) order SPR modes at the metal/ambient medium and nant wavelength with sensing RI. Based on the results
metal/fiber interfaces, respectively. that the linearly dependent coefficients R2 are 0.9999,
Moreover, with the increase of the short axis diameter 0.9996, and 0.9989 for dips A, B, and C, respectively, it
D2 of the elliptical nanohole, dip C broadens significantly can be verified that there is an excellent linear relation-
compared with dips A and B, as shown in Fig. 3c. This phe- ship between the resonant wavelength shifts and sensing
nomenon stems from the weakened coupling interaction RI. The RI sensitivity of the resonance modes is defined
between the different LSPR modes around the irregular as the resonance wavelength shift per RI unit (S = Δλ/
annular aperture and the decrease of the localized electro- Δn). Therefore, the slopes of the fitted lines are the RI
magnetic field intensity with the increase of the aperture gap sensitivities for the sensors. Figure 4b shows that the RI
width. When the short axis diameter D2 increases to 240 nm, sensitivities of dips A, B, and C are S A = 669 nm/RIU,
equaling to the long axis diameter D1, the elliptical nanohole SB = 66 nm/RIU, and SC = 526 nm/RIU, respectively. Due
turns into circular nanohole. By comparing the spectral fea- to the fact that the mode field of dip B mainly distributes
tures of the uppermost and nethermost reflection spectrum on the high RI fiber side, its sensitivity is far less than
curves in Fig. 3c, it obviously indicates that this nanodisk- that of dip A, whose mode field mostly penetrates into
in-elliptical nanohole binary array of irregular annular aper- the sensing medium layer. Another important parameter
ture can provides more excellent spectral feature than that for a biochemical sensor is the FOM, which is defined
of the nanodisk-in-circular nanohole binary array with equal as FOM = S/FWHM [17], where S is the sensitivity and
annular aperture width. Thus, the short axis diameter D2 of FWHM is the spectral linewidth of resonance dips. The

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Plasmonics

Fig. 4  a The reflection spectra evolution when the surrounding environmental RI changes from 1.33 to 1.40. b Linear relationships between the
resonance wavelength and the surrounding environmental RIs. The slopes of the fitting lines are the RI sensitivities for dips A, B, and C

above calculated sensitivities and the FWHM referred to Polarization‑Dependent Reflection Property
in the inset of Fig. 1 are used to obtain the corresponding
FOM for the three resonance modes. As a result, the FOM In the above simulations, the incident light propagating
is as high as 115.3 for dip A, while for dip C, the FOM along the z axis has a linear polarization in the x-axis direc-
is only 4.2. The ultra-high FOM of dip A is attributed tion (parallel with the long axis of the elliptical nanohole).
to the LSPR mode-coupled PSP modes with resonantly To investigate the polarization dependency of the proposed
enhanced interaction, which significantly reduces the binary array structure, the reflection spectra corresponding
radiation damping and greatly improves the local electric to the polarization angle θ from zero to 90° with a step of
field strength. Therefore, the designed CNENBA struc- 10° are calculated and provided in Fig. 5a. Here, the polari-
ture formed by introducing nanodisk into nanohole array zation angle θ is defined as the angle value of the incident
performs makes advances in sensing performance. light polarization direction relative to the x axis. As shown

Fig. 5  a The reflection spectra of the CNENBA based fiber tip versus the different polarization direction of the propagating light in fiber. b Polar
graph of the reflectivity variation at resonance wavelengths for dips A, B, and C for a 360° rotation of the polarization direction relative to x axis

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Plasmonics

in Fig. 5a, the reflection spectra indicate that the reflectance based on traditional LSPR modes. Moreover, the CNENBA
for the three resonance dips A, B, and C has their minima at structure has strong polarization-sensitive characteristics.
the initial polarization direction (θ = 0°). Then, the reflected Due to the simple structure of light and signal acquisition,
light intensity at the resonance dip position enhances with the CNENBA-based SPR fiber tip sensor is a promising
the increase of the polarization angle θ. As the polarization candidate to develop high-performance optical polarizing
direction rotates to θ = 90°, their maxima approaching to 1 devices or detection tools for remote, real-time and label-
are observed in their reflection spectra. Here, the resonance free biochemical and biomedical sensing applications.
wavelengths keep excellent consistency without obvious
shift. When the polarization angle of incident light rotates
Author Contribution Investigation, calculation, writing, C.Z.; data
one circle (from 0 to 360°) in the x–y plane, the correspond- curation, conceptualization, writing—revision and editing, X.H.;
ing polar graph of the reflectance versus the polarization reviewing, comment and revision, H.Z. All authors read and reviewed
angle is depicted in Fig. 5b. It can be seen that the reflec- the manuscript.
tance minima are observed as the polarization direction is
Funding The authors acknowledge financial support from the Youth
oriented at 0° or 180° relative to x axis. On the contrary, the Fund of the National Natural Science Foundation of China (YF-NSFC,
reflectance maxima are obtained at 90° or 270° relative to Grant No.62205383) and the Guangdong Basic and Applied Basic
x axis. It intuitively exhibits that the polarization direction Research Foundation (Grant No. 2023A1515011590).
which is parallel with the long axis of the binary structure
Data Availability All data that support the findings of this study are
would lead to severely attenuated optical reflection at three included within the article.
resonance dips. Furthermore, when the polarization direc-
tion and short axis of the binary structure are parallel, the Declarations
original three dips disappear with a shallow dip appear-
ing at the wavelength of 962 nm in the reflection spectra. Ethical Approval Not applicable.
This newly emerged resonance dip circled in red in Fig. 5a
Consent to Participate I am willing to participate in the work presented
arises from a new plasmonic resonance mode excitation in in this manuscript.
the short axis direction of the binary structure. The effects
of strong polarization dependence have a promising poten- Consent for Publication The authors have given their consent to pub-
lish this work.
tial application for polarized light detection and filters. For
the realization of the polarization sensor, it is sufficient to Competing Interests The authors declare no competing interests.
measure the intensity of the reflected light after calibration
at certain wavelengths where plasmonic resonance occurs.

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