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Bhishma Karki ,a,* Arun Uniyal ,b Tarun Sharma,c Amrindra Pal ,b and
Vivek Srivastavad
a
Tribhuvan University, Tri-Chandra Multiple Campus, Department of Physics, Kathmandu,
Nepal
b
DIT University, Department of Electronics and Communication Engineering,
Dehradun, Uttarakhand, India
c
Himachal Pradesh University, University Institute of Technology, Department of Electronics
and Communication Engineering, Shimla, Himachal Pradesh, India
d
ABES Engineering College, Department of Mechanical Engineering, Ghaziabad,
Uttar Pradesh, India
1 Introduction
The field of optical biosensors has shown rapid growth in research from the last decade.
A particular class of optical sensors, named surface plasmon resonance (SPR) biosensor, has
wide application in bio-sensing, biochemical investigations, environmental monitoring factors
such as temperature and pressure sensing, and food safety.1–7 The principle of operation of the
SPR-based biosensors is attenuated total reflection (ATR)8 upon applying an input laser beam
to the metal-dielectric interface. As a result, the energy levels of free electrons promoted from
the ground state to a higher one, giving birth to surface plasmons (SPs) having oscillations at
resonance conditions. Kretschmann and Raether9 and Otto10 configuration are two prism cou-
pling configurations employed to design SPR biosensors. But Kretschmann’s configuration is
popularly used in SPR sensors because it can be easily implemented.11,12,13 The opto-electronic
properties of two-dimensional materials (2D) such as graphene, black phosphorus (BP) to use
in the SPR-based bio-sensing design due to the sensitivity enhanced a significant factor.
Researchers follow the oxidation-reduction approach as it strongly affects the sensor’s per-
formance. Instead of single layer-based designs, multiple-layer designs are proposed using
different metal-dielectric layers giving rise to sensitivity.14–19 Different sensor designs made
earlier use Au, Ag, etc., as major choice combinations of the metal layer. Ag material in our
proposed design makes it a perfect choice than other materials such as Au due to its extraor-
dinary properties such as high molecular rate of adsorption and accuracy. The resonance curve
is narrow using the Ag metal compared to the Au metal-based biosensor.20 The resonance curve
broadened, the full width half maximum (FWHM) parameter of the sensor increases, so the sen-
sor’s performance decreases. Although the oxidation problem exists while using Ag as a metal in
SPR sensor-based designs,21 the problem is compensated with 2D material (such as BP). The Ag
metal-based sensor shows better performance.22 The biosensors are a functional integrated device
consisting of a bio-receptor and a transducer generally known as the biorecognition element. The
interaction with the analyte is done with the help of a bio-receptor. Then the change in signal after
combination with the analyte can be easily measured with a transducer. Previously some research
work is based on heterogeneous designs also using biomolecular recognition elements, which
improves the sensitivity by reducing the difficulties in fabrication.23–25
Formalin is a formaldehyde solution (∼40%) in water, used as food preservatives and dis-
infectants claimed by some researchers. So the formalin detection is a concerning issue as it is a
biochemical mechanism. Some severe diseases, such as chronic cancer, are severe issues after
frequent intake26,27 of the formalin-based preservative.
BP as a 2D material semiconductor material,28 having honeycomb lattice structure gaining
popularity in SPR sensor designs with their promising optoelectronic properties unlike the prop-
erties of graphene, MoS2 such as more incredible molecular adsorption energy,29,30 the more
excellent surface-to-volume ratio,31 direct bandgap, greater mobility, low losses in virtue of low
extinction coefficient.32,33 BP oxidizes quickly in the water.34 But the sensitivity of the SPR
sensor can be extensively improved using other materials with BP.
In addition to this, a semiconductor material proposed here in our design is indium phosphide
(InP), composed of the material indium and phosphorus. Its crystal structure is called zinc
blende.35 It has many optical properties such as direct bandgap, as its dielectric constant’s real
part is high, giving help in incident radiation absorption in the metal surface. When coupled with
Ag, it reduces the oxidation problem of metal, giving high-performance parameters and high
sensitivity, making it a suitable choice for sensor designs.36
Earlier research has been reported worldwide using different material-dielectric multilayer
SPR sensor structures. Rouf and Haque proposed a multi-layer SPR sensor design using
the combination of Au, Ag, InP, Titanium, airgap, and they calculated the values for sensitivity
factor (SF) as 70.90 deg ∕RIU and combined sensitivity factor (CSF) as 372.8 RIU−1 .
Wu et al.37 designed an SPR sensor with few layers of BP and graphene/transition metal dichal-
cogenides, compared it with a conventional Ag layer-based SPR sensor, and calculated the
sensitivity as 279 deg ∕RIU, which is 2.4 times higher than conventional biosensor.
Maurya et al. crafted a multiple-layer biosensor design (with graphene and MoS2 ) and found
that the performance parameters such as detection accuracy (DA) and quality factor showed
improvement over the conventional structure.38 Pal et al.39 demonstrated an SPR sensor using
BP as the material with Au layer, and the value of sensitivity was found to be 180 deg ∕RIU
which was better than the conventional structure (126.6 deg ∕RIU) and using graphene
material (128 deg ∕RIU). Singh and Raghuvanshi40 drafted an SPR-based gas sensor multi-
layer design using Bi-metallic Au and Bi-BP layers and achieved the sensitivity parameter as
245.5 deg ∕RIU at 633 nm. Karki et al.21 theoretically demonstrated an SPR sensor using
franckeite and graphene and bimetallic layers of Ni and Ag and achieved a sensitivity of
352 deg ∕RIU. Nisha et al.41 designed a biosensor based on Au, MoS2 , nickel, graphene and
obtained 229 deg ∕RIU sensitivity. Kumar et al.42 proposed an angular interrogation-based
SPR sensor for DNA hybridization using multi-layers of copper, germanium with graphene
and achieved detection sensitivity 165.94% higher than the conventional sensor.
The proposed paper is divided into sections as Sec. 2 spreads light on theoretical analysis
and mathematical modeling of SPR sensor design. The model consists of the metal layer
(Ag), one binary semiconductor material (InP), and one 2D material (BP) with sensing
medium using Kretschmann’s configuration with BK7 prism as a coupling prism. The
parameters such as sensitivity (S), the figure of merit (FoM) or quality factor (Q), and
DA are calculated. Section 3 explains the results and discussions. At last, Sec. 4 concludes
the paper.
μc μs
θSPR ¼ sin−1 : (1)
μp ðμc þ μs Þ
EQ-TARGET;temp:intralink-;e001;116;573
Here, μp and μs are RI of BK7 prism and sensing medium (aqueous solution), respectively.
The μc denotes the equivalent RI of Ag/InP/BP combined. The RI of a composite layer may be
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
defined by μc ¼ 3 ðμ1 μ2 μ3 Þ. For generating the SPR mechanism, matching between SPW vector
and evanescent wave vector is necessary.43
Ag 45 (t 1 )
InP P 2 (t 2 )
The refractive index of the BK7 prism is computed using the formula:8
The value of the RI of the prism is 1.5151 at λ ¼ 633 nm. The metal film’s RI is being
calculated by Drude’s method; its mathematical expression is44
λ2 λc
μ21 ¼ 1 − ; (3)
λ2p ðλc þ iλÞ
EQ-TARGET;temp:intralink-;e003;116;655
δn
Δμs ¼ μ2s − μ1s ¼ C ; (4)
δc
EQ-TARGET;temp:intralink-;e004;116;512
ution. The propagation constant of SPW alters with alteration in SPR angle given by46
2Π
kS ¼ μ sin θSPR : (5)
λ p
EQ-TARGET;temp:intralink-;e005;116;345
With the tunable angle of incidence of optical radiation, the resonance condition for SP (SPs)
will be achieved minimum for reflectance. The parameters such as reflectance using a popular
transfer matrix method (TMM) have been computed because, in this method, the approximation
is not used. Its accuracy mainly focuses on the construction of SPR sensors indicating their
dimensional parameters. Some performance parameters such as S, FoM, and DA are calculated
for the proposed sensor.
Here, R1 , S1 denotes tangential components of electric and magnetic field vectors corresponding
to the first boundary. Similarly, Rn−1 , Sn−1 symbolizes electric and magnetic field vectors at the
last boundary. The characteristics matrix for multi-layer model given as
Y
n−1
M11 M12
M¼ Mk ¼ : (7)
M21 M22
EQ-TARGET;temp:intralink-;e007;116;735
k¼2
Here
Cos ϒk −i sin ϒk ∕qk
Mk ¼ : (8)
−iqk sin ϒk cos ϒk
EQ-TARGET;temp:intralink-;e008;116;681
rffiffiffiffiffiffiffiffiffiffiffiffi
ffi
μk
Here, qk ¼ cos θk and ϒk ¼ nk 2πλ cos θk dk
Єk
The value of reflectance comes out to be, Rp ¼ jr2123 j using the above method, here rp , reflec-
tion coefficient expressed as46
ϵ 1 k2 − ϵ 2 k1
r12 ¼ ; (9)
ϵ 2 k1 þ ϵ 1 k 2
EQ-TARGET;temp:intralink-;e009;116;584
ϵ 3 k2 − ϵ 2 k3
r23 ¼ ; (10)
ϵ 3 k2 þ ϵ 2 k 3
EQ-TARGET;temp:intralink-;e010;116;528
y is incident magnetic field amplitude and rp is the reflection coefficient. P1 ðzÞ is the
Here H inc
filed at the first layer, and given as
cosðβkðat zÞ Þ i∕q1 sinðβkðat z Þ
P1 ðzÞ ¼ : (11)
iqj sinðβkðat z Þ cosðβkðat z Þ
EQ-TARGET;temp:intralink-;e011;116;735
Similarly, the electric and magnetic distribution in the layer j ≥ 2 with the help of the fol-
lowing expressions:
Y1
H yj ðzÞ 1 þ rp
¼ Pj ðzÞ Pi ðz ¼ zi þ di Þ H inc ; zj ≤ z ≤ zjþ1 ; (12)
−Exj ðzÞ q1 ð1 − rp Þ y
EQ-TARGET;temp:intralink-;e012;116;675
i¼j−1
Consistent with Fig. 1 in the manuscript, the substrate and ambient will represent the analyte
and prism, respectively, when the basic structure shown in Fig. 2 is used to create an SPR sensor.
It clearly shows how the incident, reflected, and transmitted waves are affected while passing
through the structure.
Case 1: For P ¼ 0, B ¼ 0
Figure 3(a) gives a view of the case of a conventional sensor having no layers of InP (P ¼ 0)
and BP (B ¼ 0). The reflectance curve is shown here, indicating a sharp dip in resonance in
the vicinity of certain angles of incidence, showing adsorption efficiency of the SPR sensor for
incident radiation, which produces SPs. The change in SPR resonance angle, δθ ¼ 1.165 deg
for two resonance curves at RI. 1.33 and 1.34, is observed. The sensitivity calculated for this
sensor is 116.5 deg ∕RIU.
Case 2: For P ¼ 0, B ¼ 1
Further modifications in conventional structure by adding a single BP layer and no InP layer
(P ¼ 0 and B ¼ 1) with all parameters are the same as case 1 shown in Fig. 3(b). The increase in
Fig. 2 Plane-wave interaction with a multilayer system made up of three homogeneous and iso-
tropic media with four interfaces separated by two semi-infinite homogeneous, isotropic, and
dielectric media.
Fig. 3 Graph between reflectance and incidence angle at RI = 1.33 and 1.34 (a) For P ¼ B ¼ 0;
(b) For P ¼ 0, B ¼ 1; (c) For P ¼ 1, B ¼ 0; and (d) For P ¼ B ¼ 1.
values of resonance offset shift, δθ ¼ 1.187 deg, and sensitivity as 118.7 deg ∕RIU is observed
compared with traditional case (P ¼ 0, B ¼ 0). This advancement in the values of resonance
curve offset dip and sensitivity confirms that the use of BP material in the structure is appropriate
due to its properties such as direct bandgap with greater mobility, making it suitable for design-
ing multilayer SPR biosensors.
Case 3: For P ¼ 1, B ¼ 0
In this scenario, a single layer of InP is introduced with no layer of BP, i.e., P ¼ 1 and B ¼ 0;
it further increases both resonances offset dip and sensitivity, giving values 1.311 deg and
131.1 deg ∕RIU, respectively [shown in Fig. 3(c)]. This advancement in both parameters’ values
compared to previous cases is due to the properties of InP, such as the absorption rate of incident
light in the metal layer is high due to its high real part dielectric constant. Due to this, more shift
in the resonance angle is obtained in the resonance angle. A large excursion is obtained in the
resonance curve, the sensitivity of the sensor goes high.
Case 4: For P ¼ 1, B ¼ 1
This case evaluates the proposed sensor’s performance using both materials (InP and BP)
single layer (P ¼ B ¼ 1). The amount of shift and resonance curve dip is noted here signifi-
cantly, and the improvement in the drift in resonance angle δθ ¼ 1.337 and sensitivity S ¼ 133.7
is computed as shown in Fig. 3(d). Finally, after studying all four cases, it is concluded that the
sensor’s performance is maximum in this case; the monolayer of InP and a monolayer of BP
are used.
Fig. 5 Plot giving the relation between Sensitivity and RI of sensing layer.
Fig. 6 Impact of Incidence angle on reflectance (a) taking single layer of InP and varying BP layers
from 1 to 16 and (b) varying InP layers (1 to 4) and a single layer of BP.
in sensor sensitivity with multi sheets of BP and InP, respectively. Figure 6(a) shows an increase
in reflectance with variation in the angle of incidence, taking constant RI. as 1.33. The sharp dip
in reflectance shifts to a greater angle of incidence, making the SPR curve change its shape from
narrow to broad with the increasing number of BP layers (1 to 16) with a gap of 4 with each layer.
In continuation to this, Fig. 6(b) shows the effect on sensitivity by varying the InP layers with no
change in layers of BP. As in the earlier case, dip in reflectance shifts to a greater angle of
incidence with making SPR curve overall with respect to increase in the number of InP layers
(1 to 4).
For higher B and P ≥ 2, performance analysis is somehow complex due to the transfer of
resonance curves for different RI. values of sensing medium overlapping.
The thickness of the Ag metal has been optimized. The study considers the metal layer (Ag)
thickness variation from 30 to 50 nm, and the minimum reflectance observed is 0.00589 with
50 nm thickness of silver layer as shown in Fig. 7. The corresponding values of Rmin for the silver
layer thicknesses of 30, 35, and 40 nm are 0.56517, 0.4022, and 0.023022, respectively. As we
increase the thickness of the silver layer, further dip resonance curves are also noted. The opti-
mized thickness of 45 nm of the Ag metal has been taken.
The parameters such as the thickness of a silver layer, the refractive index of the sensing
medium, and the number of BP layers may affect the performance of the SPR sensor. The sen-
sitivity and minimum reflectance values should be high and low for higher sensor performance,
respectively. In Fig. 8, the number of BP layers varies from 0 to 9, and its impact on reflectance is
observed for the optimized thickness of silver taken as 30, 35, 40, 45, and 50 nm. The lowest
value at which reflectance occurs is called the angle of resonance. The InP layer thickness is
Fig. 7 Incidence angle versus reflectance curve for silver layer thickness (Ag = 30 to 50 nm).
Fig. 8 Reflectance alterations with BP layers for various silver layer thicknesses.
fixed at 2 nm. At the metal-dielectric interface, SPs get excited, and finally, as a result, a drop in
the reflectance curves is observed, giving drops in reflectance angle. The reflectance continu-
ously increases for the Ag layer (40, 45, and 50 nm). For Ag (30 nm), the reflectance contin-
uously decreasing and at last Ag (35 nm), the reflectance first decreases then increases after eight
layers of BP.
Figure 9(a) shows electric field distributions regarding average distance from interfaces (Ag-
InP-Sensing medium layers). For this modified conventional design plot, no BP layer is present.
The electric field distribution increases exponentially between Ag-InP and InP-sensing media
interfaces and decreases exponentially after InP-sensing media’s final interface. Figure 9(b)
Fig. 9 Electric field distribution w.r.t. distance from prism for (a) Ag-InP-SM nanosheets and
(b) Ag-InP-BP-SM nanosheets.
Au+MoS2+Au+Graphene 182 — — 50
Au+TMDC+Au+Mxene 198 — — 51
Au+MoS2+Ni+Graphene 229 — — 39
gives the electric field plot for the proposed SPR sensor design. At the metal-dielectric interface,
a high magnitude evanescent field wave is generated because of SPs excitations, exponentially
decaying at an average distance from the interface of metal-dielectric.1
Table 4 shows the comparative analysis of the earlier reported work. The proposed sensor is
ultra-sensitive for the RI change.
4 Conclusion
A hybrid SPR biosensor based on the InP with 2D BP is proposed for formalin detection in
water. The design incorporates optimized Ag, InP, and BP layers with 45, 2, and 0.34 nm, respec-
tively. The thickness of the InP and BP layers impacts the biosensor’s sensitivity. The biosensor
had a maximum sensitivity of 250.2 deg ∕RIU when three layers of InP and one BP layer were
considered. It is worth noting that the proposed systems have a sensitivity that is 2.15 times
higher than traditional Ag-based sensors. The BP and InP have exclusive optoelectronic proper-
ties such as high surface-to-volume ratio, direct bandgap, and higher molecular adsorption, mak-
ing them suitable for formalin detection applications.
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serving in the National Research Council as an executive chairman. He has published more than
31 research papers in theoretical physics, catalysis, optics, plasmonics, nanotechnology, and
materials chemistry.
Arun Uniyal is a research scholar at DIT University, Dehradun, Uttarakhand, India. His current
research interest includes SPR biosensors, photonics, etc. He received his BTech degree in elec-
tronics engineering from Kurukshetra university in 2008, and MTech degree in wireless mobile
communication from Uttarakhand technical university in 2012. He has over eight years of teach-
ing experience in the electronics and communication engineering department and has published
five research papers in the wireless communication engineering field.
Tarun Sharma received a master’s degree in communication systems from Guru Nanak Dev
University in 2009 and his PhD degree in the hybrid plasmonic waveguide from Thapar
University in 2016. He was a postdoctoral fellow with the School of Electrical Engineering,
Korea Advanced Institute of Science and Technology, South Korea. He was also a postdoctoral
fellow with the Centre for Nano Science and Engineering, Indian Institute of Science, Bengaluru.
He is currently working as an assistant professor Electronics and Communication Engineering.
University Institute of Technology, Himachal Pradesh University, Shimla, India. His current
research interests include nanophotonics integrated circuits, hybrid plasmonic waveguides, and
silicon photonics.
Amrindra Pal has completed his BTech in ECE from Uttar Pradesh Technical University,
Lucknow in 2008, ME degree in Electronics Instrumentation and Control from Thapar
University, Patiala in the year 2013, and PhD in the field of design and modelling of opto-
electronics devices from DIT University, Dehradun in the year 2018. He is working as an
assistant professor in the School of Engineering and Technology in the EECE Department,
DIT University, Dehradun, India. He has published 50 papers in international journals and
international conferences. His research interest includes integrated optics, plasmonics, opto-elec-
tronics devices, electro-optics, optical biosensor, and RF and microwave.