Sensors and Actuators B 207 (2015) 117–122

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Sensors and Actuators B: Chemical

journal homepage: www.elsevier.com/locate/snb

On the electric field enhancement and performance of SPR gas sensor

based on graphene for visible and near infrared
Pradeep Kumar Maharana a , Rajan Jha a,∗ , Punnag Padhy b
a
Nanophotonics and Plasmonics Laboratory, School of Basic Sciences, Indian Institute of Technology Bhubaneswar, Toshali Bhawan, Bhubaneswar, Odisha,
India
b
School of Electrical Sciences, Indian Institute of Technology Bhubaneswar, Toshali Bhawan, Bhubaneswar, Odisha, India

a r t i c l e i n f o a b s t r a c t

Article history: We propose a high performance surface plasmon resonance (SPR) affinity gas sensor based on graphene
Received 12 June 2014 on Ag in visible and near infrared. Proposed sensor configuration has been optimized for maximum
Received in revised form 2 October 2014 surface plasmon field at the sensing layer interface. The field intensity enhancement factor at sensing
Accepted 5 October 2014
layer interface is found to be higher than that of silicon over layer on Ag thereby increasing the imaging
Available online 12 October 2014
sensitivity by 340%, 120% and 82% and detection accuracy by 440%, 150% and 100% as compared to Si on
Ag configuration at  = 653 nm,  = 850 nm and  = 1000 nm respectively. The performance of the sensor
Keywords:
is found to be high over a broad refractive index range (1.0000–1.0008) of gaseous analyte with sensor
Biosensor
Surface plasmon resonance
resolution of 8 × 10−5 RIU and 2 × 10−5 RIU at  = 653 nm and  = 1000 nm respectively. We believe the
Graphene proposed SPR based gas sensor configuration will open a new route for efficient gas sensing by riding on
Imaging sensitivity the advantage of graphene and latest nanofabrication techniques.
Field intensity enhancement factor © 2014 Elsevier B.V. All rights reserved.

1. Introduction exponentially in the metal and dielectric close to interface. These

The ever increasing complexities in industrial processes to meet
market demands result in the emission of a host of hazardous
gaseous byproducts which are potentially harmful to human health
and the environment in general. The efficient detection mechanism
of such range of gases is very important and must be detected with
utmost accuracy. This type of efficient gaseous detection is possible
by riding on the advantages of graphene [1]. Due to the 2-D struc-
ture of graphene every carbon atom behaves effectively as a surface
atom thus making it highly sensitive to adsorbed gaseous molecules
[1]. Its high electron mobility at room temperature makes it an
ideal candidate for real time sensing applications. The above advan-
tages of graphene can be efficiently harnessed for designing and
developing surface plasmon resonance (SPR) based gas sensors.
SPR is a simple, direct, real time and sensitive optical sensing
technique used for probing refractive index changes in the vicinity
of a thin metal film. It is observed when a p-polarized light is inci-
dent on the metal surface in which the conduction band electrons
are approximated as free electron plasma [2]. Due to the incident p-
polarized light there is collective resonant oscillation of these free
electrons at the metal–analyte interface. This is characterized by a
propagating charge density wave along the interface that decays
∗ Corresponding author. Tel.: +91 6742576100.
E-mail addresses: rjha@iitbbs.ac.in, rajaniitd@gmail.com (R. Jha).
collective oscillations of electrons are called as surface plasmon
(SPs) and are sensitive to any refractive index alteration in the
dielectric medium adjacent to metal surface [3]. When the wave
vector of SP matches with the parallel component of wave vector
of incident light, it results in a sharp dip in reflectance spectra as
per the resonance condition shown below in Eq. (1).
  ε ε 1/2 
2 2 m d
np sin spr = Re (1)
o o εm + εd
Here  spr is the resonance angle, np is the refractive index of prism,
εd and εm are the dielectric constant of sensing medium and SPR
active metal respectively and o is the operating wavelength.
Ever since the use of SPR sensor for gas detection by Lied-
berg and co-workers [4], this optical technique has drawn growing
attention in the field of high performance gas sensing down to
single molecular level [5–9]. Several innovative techniques have
been proposed to enhance the performance of the SPR sensor by
optimizing the full width at half maximum (FWHM) and the shift
in the resonance angle (or wavelength) of SPR curves [10–20].
Recently, it has been found that coating the metal surface with
high index material enhances the evanescent field at metal–analyte
interface [12,21,22]. Silicon (Si) as high index prism has been
used for sensing but Si over layer is prone to aging effect due to
oxidation of silicon which results in the broadening of full width

http://dx.doi.org/10.1016/j.snb.2014.10.006
0925-4005/© 2014 Elsevier B.V. All rights reserved.
118 P.K. Maharana et al. / Sensors and Actuators B 207 (2015) 117–122

Fig. 1. Schematic of proposed set up of SPR gas sensor.

at half maximum (FWHM) of SPR curve thereby degrading the sen-
sor performance [23]. We have addressed the above limitation by
using graphene as the dielectric over layer on Ag because it has
been found that graphene not only prevents oxidation of Ag [24],
but itself is robust against oxidation [25,26]. Moreover, our results
show that the graphene over layer on Ag shows exceptionally high
performance as compared to silicon over layer in imaging mode of
interrogation [27,28]. Unlike the conventional angular interroga-
tion technique, in imaging mode, the spatial change in reflectivity
is measured at a fixed incident angle, i.e. without any moving com-
ponents which guarantees a simpler design from implementation
point of view. The imaging sensitivity is mathematically defined
as (dR/dnd ) which quantifies the change of slope of the reflectivity
curve close to resonance angle ( spr ) [27]. Greater the slope better is
the imaging sensitivity. This can be observed from the performance
analysis of the proposed sensor as shown in Fig. 1.
2.2. The wavelength dependent dielectric constant of metal and
graphene
The wavelength dependence of dielectric constant of metal layer
follows Drude Lorentz model as given in below equation:
2 c
εm () = −εmr + iεmi = 1 − (3)
2p (c + i)
where  is the wavelength in ␮m, p and c denote the
plasma wavelength and collision wavelengths respectively. The
values of p and c for Ag are respectively 1.4541 × 10−7 m and
1.7614 × 10−5 m [10,29]. Further, the refractive index of graphene
in the range 210–1000 nm has been taken from Ref. [30].

2. Design consideration and theory 2.3. Numerical formulation of reflectivity (R)

The present configuration is a four layer planar structure, con- We employed the well known transfer matrix method [29] to
sisting of SF11 prism, Ag, graphene and flow cell containing gas obtain the reflectivity from the proposed SPR sensor, as discussed
as analyte as shown in Fig. 1. Optimized thickness of Ag film below. Different layers (i.e., silicon prism–metal–graphene-sensing
and graphene can be successively deposited on the prism surface layer) of thickness dk , dielectric constant εk , and refractive index nk
by suitable deposition techniques for efficient SP excitation. TM- are assumed to be stacked along the Z-axis. The tangential fields at
polarized light is to be incident on the prism–metal interface at the first boundary Z = Z1 = 0 are related to those at the final boundary
angles beyond critical angle and the reflected light can be col- Z = ZN−1 by
lected and studied using photo detector. Here, N-layer model has
been considered for theoretical calculation of reflectivity of TM-    
polarized light [29] from the multilayer structure to study the U1 UN−1
=M (4)
device performance. In the following we discuss the dispersion of V1 VN−1
different constituents and the numerical formulation of reflectivity
along with the performance parameter of the proposed sensor.
where U1 and V1 , respectively, are the tangential components of
2.1. The wavelength dependent refractive index of SF11 electric and magnetic fields at the boundary of first layer. UN−1 and
VN−1 are the corresponding fields at the boundary of Nth layer and
The refractive index of SF11 is given by M is known as characteristic matrix of the combined structure. It is
to note that the SPP modes are p-polarized, so for p-polarized light
1.737596952 0.3137473462
n2 = 1 + + 2 M is given by:
2 − 0.013188707  − 0.0623068142
1.898781012
 
+ (2) 
N−1
M11 M12
2 − 155.23629 M= Mk = (5)
M21 M22
where  is the wavelength in ␮m. k=2
 P.K. Maharana et al. / Sensors and Actuators B 207 (2015) 117–122 119

with
 
cos ˇk (−i sin ˇk )/qk
Mk = ,
−iqk sin ˇk cos ˇk

1/2
where qk = (εk − n21 sin2 1 ) /εk , and ˇk =
2
(2dk /) εk − n21 sin 1 .
The parameter  1 is the incident angle at the prism base (in
radians). Thus, transfer matrices are calculated using above equa-
tions. The four elements M11 , M12 , M21 and M22 of matrix M are
used to calculate the amplitude reflection coefficient (r), which for
p-polarized incident light is given as:
(M11 + M12 qN )q1 − (M21 + M22 qN )
r= (6)
(M11 + M12 qN )q1 + (M21 + M22 qN )
Finally, the reflectivity (R) for p-polarized light is given by:

R = |r|2 (7)

2.4. Performance parameter

The well known angular interrogation technique is known to be

robust and sensitive because commercially available instrumenta-
tions allow angular resolutions as low as 0.001◦ . However, a severe
limitation of this scheme is that the scanning angle type cannot
provide the capability of screening diverse sets of biomolecular
interactions at a time [27,28]. On contrary to this scanning angle
type SPR imaging scheme measures the spatial changes in reflectiv-
ity at a fixed incident angle, i.e. without moving any component and
indeed, this unique property offers an attractive tool for monitoring
numerous interactions in a parallel manner [27,28]. Therefore, the
performance of the SPR imaging sensor can be defined as below.
Since, the reflectivity (R) significantly changes with the change
in the refractive index of the sensing medium, therefore, large
change in R would lead to high sensitivity. If the refractive index of
the sensing layer is altered by dna and the corresponding change in
the reflectivity is dR, then the sensitivity of a SPR sensor is defined
in terms of imaging sensitivity as follows:
dR
S=
dna
As discussed earlier, the full width at half minimum (FWHM)
corresponding to the SPR curves (ı 0.5 ) should be as small as pos-
sible so that the error in determining the reflectance is minimum.
Thus, the detection accuracy (DA) of SPR sensor is the reciprocal of
full width at half maximum (FWHM = ı 0.5 ) i.e.
1
DA =
FWHM
High detection accuracy results from narrower FWHM which
in turn helps in accurate measurement. Therefore, for high perfor-
mance of any sensor the imaging sensitivity and detection accuracy
should be as high as possible.
3. Results and discussion
The SP field distribution at sensing layer interface largely affects
the overall performance of SPR based sensor through overlap
integral between the evanescent field of SPs (F(r)) and spatial dis-
tribution of dielectric constant (εd (r)) of the sensing region in three
dimensional space i.e. overlap volume [31]. The reflectivity from
proposed multilayer system is proportional to this overlap volume
and accordingly the sensitivity of SPR sensor is proportional to over-
lap integral [31]. The sensitivity of the sensor increases whenever
there is increase in numerical value of overlap integral. Enhancing
SP field at sensing layer interface is a novel approach to increase the
Fig. 2. (a) One dimensional plot of absolute magnetic field intensity as a function
of distance normal from interface for silicon (10 nm) on Ag (43 nm) configuration
and (b) two dimensional plot of magnetic field intensity distribution as a function
of distance normal from interface for silicon (10 nm) on Ag (43 nm) configuration at
nd = 1.0000 and  = 653 nm.
numerical value of overlap integral. For numerical study, we have
(8)
considered three different wavelengths i.e. 653 nm, 850 nm and
1000 nm. For these operating wavelengths, 43 nm of Ag film, 10 nm
of Si layer, 0.34 nm of monolayer graphene sheet and sensing layer
refractive index of 1.0000 have been considered. Figs. 2(a) and 3(a)
show the one dimensional plot of absolute value of magnetic
field intensity of SP parallel to interface as a function of distance
normal to interface for Si (10 nm) on Ag (43 nm) and graphene
(9) (0.34 nm) on Ag (43 nm) configuration respectively for sensing
layer refractive index (nd ) of 1.0000 and operating wavelength
653 nm. These SP fields have been calculated using finite element
method (FEM). The magnitude of these fields are 825 (A/m)2 and
375 (A/m)2 at graphene–sensing layer interface and Si–sensing
layer interface respectively. In order to substantiate the results of
Figs. 2(a) and 3(a), Figs. 2(b) and 3(b) illustrate the two dimen-
sional plot of magnetic field intensity distribution with distance
normal to interface. Such high magnetic field at graphene–sensing
layer interface compared to Si–sensing layer interface have corre-
sponding high electric field intensity and in turn can help to achieve
high performance SPR gas sensor. Taking the advantage of this high
electric field intensity, all the analysis and the results have been
obtained for graphene on Ag configuration. The optimized Ag thick-
ness is found to be 43 nm for which all the incident energy gets
coupled to SP wave showing almost zero reflectivity at the reso-
nance angle 35.71◦ of SPR curve. Also, from the SPR curve, we found
that FWHM is significantly low (0.609◦ ) thereby indicating high
detection accuracy (inverse of FWHM), an important parameter for
120 P.K. Maharana et al. / Sensors and Actuators B 207 (2015) 117–122
Fig. 3. (a) One dimensional plot of absolute magnetic field intensity as a function of
distance normal from interface for graphene (0.34 nm) on Ag (43 nm) configuration
and (b) two dimensional plot of absolute magnetic field intensity as a function of
distance normal to interface for graphene (0.34 nm) on Ag (43 nm) configuration at
nd = 1.0000 and  = 653 nm.
designing high performance SPR sensor. Further to understand the
low FWHM of such system, we study the effect of different number
of graphene layer on the width of the SPR curve. Fig. 4 illustrates the
variation of reflectivity with incident angle for different number of
graphene layers (L = 1, 3, 5, 7 and 10) for optimized Ag thickness
and nd = 1.0000. As can be seen from Fig. 4, the FWHM are 0.609◦ ,
0.740◦ , 0.893◦ , 1.069◦ and 1.384◦ for L = 1, 3, 5, 7 and 10 respec-
tively. We observed that FWHM increases with number of graphene
layers thereby decreasing the detection accuracy and hence
Fig. 4. Variation of reflectivity as a function of incident angle for different graphene
layers at nd = 1.0000 and  = 653 nm.
Fig. 5. Variation of electric field intensity enhancement factor as a function of dis-
tance normal to graphene–sensing layer interface for different number of graphene
layers at nd = 1.0000 and  = 653 nm.
affecting the performance of the sensor. This increase in FWHM
with graphene layers is due to the increase in damping of SP
oscillation because of finite imaginary part of dielectric constant
of graphene [11,32]. SPR curve broaden for higher number of
graphene layers, as the concentration of SPs inside graphene mul-
tilayer increases due to their increased penetration depth resulting
from increased in plane wave vector of SP. Hence, SPs exhibit
damped oscillation and the FWHM is a linear function of damp-
ing, so FWHM increases with increasing the number of graphene
monolayer which leads to wider curves. We also observed that
with increasing number of graphene layer, resonance angle is red
shifted and the SPR curve gets broader and shallower. This influ-
ences the SP field distribution at the sensing layer interface and
affects the performance. To study the effect of graphene layers
on SP field distribution at the interface, we plotted the electric
field intensity enhancement factor (FIEF) with distance normal to
graphene–sensing layer interface for different number of graphene
layer at nd = 1.0000 as shown in Fig. 5. Mathematically, FIEF is
equal to the ratio of the square of the field at graphene–sensing
layer interface to the incoming intensity (square of the field) at the
prism–metal interface, for p-polarized light. Therefore, the FIEF at
graphene–sensing layer interface can be obtained by relating the
electric field to magnetic field as per Eq. (10) [29]:
2 2
E|| (N/N − 1) ε1 Hy|| (N/N − 1)
= (10)
E|| (1/2) εN Hy|| (1/2)
It can be seen from Fig. 5, that the FIEF at the interface decreases
from 112 at L = 1 to 31.3 at L = 10. The decrease in FIEF with num-
ber of graphene layer is due to the increased damping within
graphene multilayer [32]. This reduced FIEF would result in per-
formance degradation of the sensor. Hence, one has to consider
the minimum number of graphene layers on Ag for optimal perfor-
mance. One can observe from Fig. 5 that FIEF decays exponentially
with distance normal from the graphene–sensing layer interface
[29] thereby showing that SPR sensor with proposed configura-
tion is strongly sensitive to any alteration in the sensing medium.
Since FIEF at graphene–sensing layer interface is a measure of
sensitivity, so Fig. 6(a)–(c) shows the variation of imaging sensi-
tivity with gas refractive index nd over a broad wavelength range.
The solid green curve represents imaging sensitivity for graphene
monolayer on Ag. As can be seen from Fig. 6(a) that the imag-
ing sensitivity of the proposed probe is as high as 122.18 RIU−1 at
nd = 1.0000 and decreases to 121.9 RIU−1 at nd = 1.0008. However,
at higher wavelength  = 850 nm (Fig. 6(b)) the imaging sensitiv-
ity increases to 332.5792 RIU−1 at nd = 1.0000 and 331.765 RIU−1
at nd = 1.0008. Further at  = 1000 nm, the imaging sensitivity
increases to 455.3611 RIU−1 at nd = 1.0000 and to 454.2559 RIU−1
 P.K. Maharana et al. / Sensors and Actuators B 207 (2015) 117–122
Fig. 6. Variation of imaging sensitivity as a function of sensing layer refractive index
(1.0000–1.0008) at (a)  = 653 nm, (b)  = 850 nm and (c)  = 1000 nm. Inset shows
the variation of imaging sensitivity with incident angle for nd = 1.0000 and 1.0008.
at nd = 1.0008 as shown in Fig. 6(c). It can be observed that imaging
sensitivity increases with the wavelength. Moreover, at  = 653 nm,
 = 850 nm and  = 1000 nm, our numerical result shows that the
values of imaging sensitivities are respectively 340%, 120% and 82%
higher as compared to high index Si over layer on Ag configu-
ration highlighting the high imaging sensitivity of the proposed
sensor over a broad wavelength range. This high imaging sen-
sitivity with graphene monolayer originates from higher FIEF at
graphene–sensing layer interface. The different inset of Fig. 6(a)–(c)
shows the variation of imaging sensitivity with incident angle
at nd = 1.0000 and 1.0008. It is to be noted that over a large
range of refractive indices (such as 1.0000–1.0008) of the gases
(N2 , O2 , H2 , CO, CO2 , O3 , CH4 , He, C3 H8 ), the variation of imag-
ing sensitivity is marginal thereby predicting a broad operating
range of the sensor with high performance over a broad wave-
length range. The marginal variation in the imaging sensitivity is
because with the increase in the value of nd , propagation vector
of SPs increases, which in turn increases the concentration of SP
fields in the lossy sensing layer thereby creating more damping
in SP oscillations and hence FWHM increases with nd . Marginal
increase in FWHM with nd thus leads to small decrease in imag-
ing sensitivity as it is a measure of slope of SPR curve. Besides
imaging sensitivity, the other important parameter of sensor is
its FWHM. Fig. 7(a)–(c) illustrates the variation of FWHM with nd
121
Fig. 7. Variation of FWHM as a function of sensing layer refractive index
(1.0000–1.0008) at (a)  = 653 nm, (b)  = 850 nm and (c)  = 1000 nm. Inset shows
variation of SPR reflectivity with incident angle for nd = 1.0000 and 1.0008.
for monolayer of graphene on Ag for  = 653 nm,  = 850 nm and
 = =1000 nm. As can be seen from Fig. 7(a)–(c), FWHM increases
linearly with increase in the value of nd . At  = 653 nm, FWHM
increases from 0.6269◦ at nd = 1.0000 to 0.6287◦ at nd = 1.0008.
However, for wavelength in near infrared regime i.e. at  = 850 nm,
FWHM varies from 0.200◦ at nd = 1.0000 to 0.2026◦ at nd = 1.0008
and at  = 1000 nm, FWHM varies from 0.1428◦ at nd = 1.0000 to
0.1444◦ at nd = 1.0008. At higher wavelength, the SPR curve is blue
shifted and the width of SPR curves decreases due to reduced
ohmic losses [2]. Based on FWHM calculation, at  = 653 nm, the
detection accuracy (DA) decreases (i.e. increase of FWHM) from
1.5951 degree−1 at nd = 1.0000 to 1.5905 degree−1 at nd = 1.0008.
At higher wavelength  = 850 nm, DA decreases from 5 degree−1
at nd = 1.0000 to 4.935 degree−1 at nd = 1.0008 and at  = 1000 nm
DA decreases from 7.002 degree−1 at nd = 1.0000 to 6.925 degree−1
at nd = 1.0008. Increasing nd , increases damping in SP oscillations
and hence FWHM increases. The inset of Fig. 7 shows the typical
SPR reflectance curve at nd = 1.0000 and 1.0008 for the respective
wavelength. It can be observed that FWHM increases marginally
with nd thereby maintaining nearly constant detection accuracy
over a broad range (0.0008) of sensing layer refractive index. Our
calculation shows that the proposed sensor has detection accuracy
440%, 150% and 100% higher as compared to Si on Ag configuration
at  = 653 nm,  = 850 nm and  = 1000 nm respectively over a broad
122 P.K. Maharana et al. / Sensors and Actuators B 207 (2015) 117–122
range of refractive indices (1.0000–1.0008) of gaseous analyte in
visible and near infrared wavelength regime. It is to be mentioned
here that the proposed sensing scheme may be utilized beyond
1000 nm wavelength, subject to the availability of the dispersion
features of the all the constituent materials of the sensor. However,
with increasing wavelength, the coupling between electromagnetic
fields and free charge carrier decreases.
4. Conclusion
The performance of the graphene based SPR gas sensor has
been numerically calculated and analyzed over a broad wave-
length range. The graphene over layer not only enhances the FIEF
at graphene–sensing layer interface to a high value but also pre-
vents oxidation of Ag. For the proposed sensor, we found that high
electric field enhancement factor thereby increases the imaging
sensitivity by 340%, 120% and 82% and increases detection accuracy
by 440%, 150% and 100% as compared to Si on Ag configuration at
653 nm, 850 nm and 1000 nm respectively. Moreover, the high per-
formance of the proposed sensor is maintained over a wide range
of sensing layer refractive index. Based on a typical safe assumption
that a 1% change in reflected intensity can be detected reliably, our
proposed sensor shows resolution of 8 × 10−5 RIU and 2 × 10−5 RIU
at operating wavelength of 653 nm and 1000 nm respectively. The
proposed graphene on Ag configuration has two fold benefits as
compared to highly reported high index dielectric over layer con-
figuration based SPR gas sensor. Firstly, the high field confinement
at graphene–sensing layer interface helps in enhancing sensitivity
as well as detection accuracy compared to reported high index Si
over layer configuration. Secondly, imaging sensing as measure-
ment scheme helps in monitoring numerous gaseous interactions
in a parallel manner. The proposed configuration may provide a
new window for designing high performance SPR sensor for gas
sensing applications by riding on the advantages of 2-D materials
like graphene and latest nanofabrication techniques.
Acknowledgements
The present work is partially supported by the Department
of Science and Technology (DST), India under project SR/FTP/PS-
086/2010. One of the author, Mr. Pradeep Kumar Maharana thanks
the group members of Nanophotonics and Plasmonics Laboratory
for their discussions and support.
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Biographies
Pradeep Kumar Maharana received M. Tech degree in Solid Sate materials (Physics)
from IIT Delhi in 2005. Since January 2011, Mr. Maharana is a full time Ph.D. student
at the School of Basic Science (Physics), Indian Institute of Technology Bhubaneswar.
Rajan Jha received his M.Sc. and Ph.D. degree from Indian Institute of Technology
Delhi, India in 2001 and 2007 respectively. From early 2008 to July 2009, he was
a post doctoral researcher at ICFO – The Institute of Photonics Sciences, Barcelona,
Spain. He was awarded JSPS (Japanese Society for Promotion of Science) fellowship
in 2009 and DAAD fellowship in 2013. He is an Associate of Indian Academy of
Sciences, Bangalore. He is currently working as Assistant Professor of Physics in
School of Basic Sciences at Indian Institute of Technology Bhubaneswar, India. He is
a regular member of Optical Society of America (OSA) and is a life member of Optical
Society of India (OSI). His areas of research are optical fiber sensors, waveguide and
interferometer. He has published more than 45 research articles including a review
article in international journals of repute.
Punnag Padhy received B.Tech. degree in electrical sciences from IIT Bhubaneswar
in 2014. He is currently working as a summer research fellow at TIFR Mumbai.