J Mater Sci: Mater Electron (2024) 35:173

Perspectives of dielectric and A.C. conductivity

behavior of MWCNT and graphene‑doped
amorphous Selenium thin films
Sachin Kumar Yadav1, S. S. Fouad2, H. E. Atyia2, and N. Mehta1,*

1
Department of Physics, Banaras Hindu University, Varanasi 221005, India
2
Department of Physics, Faculty of Education, Ain Shams University, Cairo 11566, Egypt

Received: 28 August 2023 ABSTRACT

Accepted: 19 December 2023
© The Author(s), under
exclusive licence to Springer
Science+Business Media, LLC,
part of Springer Nature, 2024
In the current study, we have focused on the dielectric and A.C. conductivity
behavior in thin films of Se:Graphene and Se:MWCNTs nanocomposite samples
by doping graphene and MWCNT in g-Se. The thin films of aforesaid nano-
composites have been prepared by physical vapor deposition. The well-known
Meyer–Neldel rule and Jonscher’s Universal power law have been employed to
investigate the variation of A.C. conductivity with frequency and temperature.
The strong dependence of conductivity over temperature is described using a
model that is applied for correlated barrier hopping (CBH) in Se:MWCNTs thin
films. However, the non-overlapping small polaron tunneling (NSPT) model is
found to be applicable for Se:Graphene thin film. The activation energy for the
nanocomposite thin films was evaluated from the Arrhenius plot. The random
free energy barrier hopping model explains the system’s ac conductivity (σac). In
our study, we observed the Meyer–Neldel rule (MNR) as well as reverse MNR
for Se:Graphene and Se:MWCNTs nanocomposite thin films, respectively. The
investigation of dielectric loss confirms that the theory of Guintini regarding
dielectric dispersion applies to our samples.

1 Introduction low loss tangent values simultaneously because of the

Since their discovery, synthetic allotropic forms of
carbon nanofillers, carbon nanotubes [CNTs], and gra-
phene-doped dielectric thin films have attracted and
inspired physicists due to their conductive properties,
capability of energy storage, and applications in wear-
able electronic devices [1–3]. However, carbon nanofill-
ers are flexible and lightweight, but it is challenging to
obtain high dielectric permittivity while maintaining
interfacial polarization. Due to the buildup of charge
carriers at the interface between filler and polymer,
the MWS process takes place at the interface between
substances with varying values of permittivity and
conductivity [4]. Therefore, the interface relationship
between the fillers and the matrix of polymers can
be adjusted with the aid of chemical alteration of the
filler content for producing composites that have mini-
mal dielectric losses and high permittivity. This will

Address correspondence to E-mail: dr_neeraj_mehta@yahoo.co.in

https://doi.org/10.1007/s10854-023-11857-x

Vol.:(0123456789)
 173 Page 2 of 16
prevent MWS polarization and regulate the dielec-
tric constant. Recent years have witnessed extensive
research of amorphous chalcogenides (Se, Te) to inves-
tigate their structure, thermodynamics, and dielectric
relaxation behavior due to their unique optoelectron-
ics and photoconductive properties as the candidates
to build other functional materials such as CdSe [5]
and ­CuInSexS2-x [6] for solar cells, xerography, and
phase change memory (PCM) applications [7]. Se-
rich chalcogenides which consist of polymeric chains
of Se doped with allotropes of carbon (CNT, graphene,
and fullerenes) possess (i) a huge and precise surface
area with a high value of the aspect ratio for chemical
treatment and (ii) delocalized electron system leads to
outstanding electronic and thermal properties [8, 9].
The main effort of the incorporation of the additive in
amorphous chalcogenides (a-Chs) such as g-Se is to
augment the electrical conductivity due to its metallic
character and the chirality (orientation of individual
graphene sheets), followed by creating a significant
reduction in activation energy responsible for the
electronic conduction of CNTs-doped nanocomposite
[10]. To deliver the appropriate details for applica-
tions in the field of solid-state devices, glass scientific
and technological researchers must first achieve an
in-depth understanding of the electronic conduction
in a-Chs. Zulfequar et al. and other research groups
have studied the additive effect of CNTs in the mul-
ticomponent glassy system and polymer matrix for
the dielectric phenomenon and thermal properties
by changing their local structure, conduction mecha-
nism over the incorporation of CNTs in the host glassy
network [11]. A nanocapacitor model (adjacent con-
ductive filler as conductors surrounded by insulating
layers of the amorphous matrix as a nanodielectric) is
employed to elucidate the high permittivity of conduc-
tive filler/polymer nanocomposite [12]. The thermo-
mechanical and electro-optical characteristics of the
ternary CNT-doped glassy composite of ­Se85Te10Ag5
were explored by some researchers in [13, 14]. They
reported the augmented electrical conductivity and
microhardness after the incorporation of CNT because
of the increased cross-linked CNT-CNT inner nano-
tube percolation network. Xia et al. [15] proposed a
theory to explain the frequency-dependent dielectric
dispersion and electrical conduction of CNT-polymer-
nanoparticle composite and showed that the addition
of nanoparticles results in an upsurge in the values of
both conductivity and permittivity. Stehlik et al. [16]
examined the influence of the addition of MWCNTs
J Mater Sci: Mater Electron (2024) 35:173
in ­AgAsS2 (CNT-AgAsS2) glass composite prepared
by the melt-quench technique and reported a signifi-
cant increase in ionic conductivity. The augment in
ionic conductivity is attributable to a reduction in
the potential barrier of the glass network for ­Ag+ ion
transport. Poh et al. [17] studied the dielectric prop-
erties of MWCNT-added epoxy thin-film composites
and observed that both dielectric constant and spe-
cific capacitance are increased drastically after the
addition of MWCNTs. Some researchers reported the
enhancement in conductivity in CuSeGeIn glasses
after CNT doping [18]. Abazine et al. noticed the dis-
persion in electrical conductivity while studying the
frequency-dependent electrical conductivity of CNT-
added polyester composites as a function of the filler
concentration of CNTs [19]. The dielectric behavior of
MWCNTs-PVDF composite with doping of CNT was
reported by Zhen et al. [20]. They observed that com-
posites having more than 5 wt % of MWCNTs exhibit
a significant dielectric absorption that may be used
in acoustic applications [20]. Mergen et al. conducted
the broadband dielectric spectroscopic experiments
of Polystyrene@graphene nanoplatelets/MWCNTs
nanocomposites and demonstrated that the existence
of carbon fillers boosted the capacitance/charge stor-
age capabilities of the sample [21]. Precise incorpora-
tion of conductive carbon filler at nanoscale resolution
in a glassy selenium network is vital for numerous
uses in sustainable energy and nanoelectronics. It is
well established that certain functional groups having
chemically bonded or substitutional doped individual
graphene layers can be used to alter the electrical char-
acteristics of selenium.
The aforementioned literature indicates that the
doping of CNT may improve the dielectric behavior
and help in raising the electrical conductivity as a
result of the delocalized unsaturated bonds of elec-
trons in MWCNTs. Such delocalization liberates the
electrons to move when an electric field is applied
[22]. Well-dispersed and properly selected nanoma-
terials can improve the insulation properties of the
composite. They act as efficient doping candidates
that may help to tailor the insulating characteristics
of the amorphous semiconductor matrix. Nanoma-
terials can be engineered to have specific dielectric
properties, allowing for the precise tailoring of the
composite’s electrical behavior. This tunability is
valuable for customizing the material to meet the
specific requirements of a given application.
J Mater Sci: Mater Electron (2024) 35:173 Page 3 of 16 173

Fig. 1  SEM images of the samples of a parent Se, b Se:MWCNTs, and c Se:Graphene

This motivated us to investigate the dielectric the thickness of the as-deposited thin films. To
behavior of nanocomposite thin films of elemental explore the dielectric behavior of the nanocom-
selenium glass with MWCNTs and graphene as a posite films, we used a two-phase nanocomposite
modifier to observe how doping affects the parent film with conducting fillers made of graphene and
g-Se. In this paper, the electron transport mechanism MWCNTs in the amorphous matrix of selenium. The
is studied by performing dielectric and A.C. conduc- SEM images and XRD patterns of the samples are
tivity measurements and the related parameters are shown in Figs. 1 and 2. The prominent diffraction
calculated following each mechanism. peaks observed at 2θ° values of 23.5° and 29.7° in
Fig. 2 correspond to the (100) and (101) reflections
of the crystalline trigonal selenium (t-Se) phase
2 Experimental [JCPDS 06-0362]. These peaks indicate the exist-
ence of crystalline structures at the nano-scale in
In this work, we synthesized amorphous thin films of the glass network of selenium embedded in the
selenium doped with MWCNTs and graphene. Proper composite material. After loading MWCNT and gra-
quantities of raw materials, i.e., 4N pure nanomateri- phene in the glass matrix, new peaks at 2θ° values
als [MWCNTs, and graphene] and 5N pure Se (Alfa of 26.9° and 43.54° indicate the presence of (002) and
Aesar; USA) were bought for the synthesis of the sam- (100) reflections of the hexagonal graphitic planes
ples. Three composite samples were produced: (i) pure and also observed very less intense peaks at 26.52°
selenium, (ii) 1% graphene-doped selenium, and (iii)
and 1% MWCNTs-doped selenium. For this purpose,
the dopant materials, graphene, and MWCNTs were
doped in selenium at 1 weight percentage.
Thin films of Se:MWCNTs and Se:Graphene (with
a fixed thickness of 200 nm) were prepared (from
the bulk sample). For the preparations of the thin
films, we used the thermal evaporation method
(E306 A, Ed wards co. England) under a high vac-
uum ~ ­1 0 –5 torr. Glass substrates were used and
hung on the substrate holder. The temperature of
the substrate holder was kept at room temperature
(303 K). For alternative current measurements, the
thin films under study were sandwiched between
two Al electrodes of sufficient thickness (500 nm,
upper and lower ). The thin films thickness was
measured using a digital thickness meter (DTM)
consisting of a quartz crystal as a sensor to monitor Fig. 2  XRD patterns of the samples of a parent Se, b
Se:MWCNTs, and c Se:Graphene
 173 Page 4 of 16
for graphene-embedded g-Se matrix. The diffrac-
tion peaks observed at 2θ° of 41.35°, 43.70°, 45.46°,
51.81°, 55.58°, and 61.37° can be accurately identi-
fied as the (110), (102), (111), (201), (112), and (202)
crystal planes of t-Se, respectively. This identifica-
tion aligns well with the JCPDS card No. 06-0362.
A programmable automatic (Fluke PM 6306) RLC
bridge was performed to directly measure the sam-
ple’s impedance (Z), capacitance (C), and dissipa-
tion factor (loss tangent or tan δ) in (1 kHz–1 MHz)
as a frequency range and at temperatures ranging
from (290 to 350 K) for the calculation of the real
part of permittivity (ε′) and electrical conductivity
(σac). The temperature dependence of the dielectric
constant (ε′) and dielectric loss (ε″) was measured
with a uniform heating rate in the temperature
span of 290–350 K. Figure 3 shows the illustration
of image main components of the test set-up. The
results of the variation in A.C. conductivity versus
applied field frequency for nanocomposite thin
films was also studied.
3 Results and discussion
Amorphous semiconductors are non-crystalline
semiconductor materials, and they exhibit unique
electrical properties compared to their crystalline
counterparts. When a small amount of conductive
filler is used as a dopant in an amorphous semicon-
ductor, it can significantly affect the dielectric prop-
erties of the material depending on various factors,
including the type and concentration of the conduc-
tive filler, the semiconductor matrix material, and
the processing conditions [23–26].
Fig. 3  Illustration of the test
set-up used for temperature Temperatures Controller & Cryostat
variation of the samples dur-
ing dielectric constant and
dielectric loss measurements
J Mater Sci: Mater Electron (2024) 35:173
3.1 Study of dielectric relaxation
The dielectric analysis of materials can examine two
fundamental aspects of electrical attributes (i) capaci-
tive insulating nature, i.e., the capacity to store elec-
trical charge, and (ii) the conduction nature, i.e., the
ability to transfer electrical charge [23]. The dielec-
tric study insights into the structure of compounds,
grain boundary, and transport properties of dielectric
material [24]. The real and imaginary dielectric permit-
tivity were plotted as a function of temperature and
frequency to study the dielectric relaxation and ther-
mally activated A.C. conduction of as-prepared nano-
composite thin films. The frequency responses of the
dielectric constant (ε′) and dielectric loss (ε″) for the
thin film of the parent sample (i.e., g-Se) are shown in
Fig. 4. From the figure, we can conclude that the die-
lectric dispersion is negligible for parent thin film and
similar results have been observed for dielectric loss.
Figure 5 depicts the temperature-dependent ε′
and ε″ for nanocomposite thin films at different fre-
quencies (1 kHz–1 MHz) and we observed similar
behavior for all investigated films. It is observed that
ε′ has weak temperature dependence at low tempera-
tures. The dielectric constant increases compared to
parent selenium thin film in the frequency range of
(1 kHz–1 MHz) while preserving low dielectric losses
for MWCNTs and graphene-doped nanocomposite
thin films respectively. Orientational polarization
is the cause of the rising trend in dielectric constant
with rising temperature. This is associated with the
thermal motion of polar molecules having mobility
increase with increasing temperature. This leads to
an increase in thermal energy that causes the rise in
the magnitude of the orientation of the electric dipoles
followed by an increment in ε′ [25–27]. To overcome
PC Setup for Data
Analysis
RLC bridge
J Mater Sci: Mater Electron (2024) 35:173 Page 5 of 16 173

Se Se
0.90 293.7 K 303.1 K
293.7 K 303.1 K 313.2 K 0.09 313.2 K 323.5 K
333.5 K 343.5 K
0.80 323.5 K 333.5 K 343.5 K

0.06
0.70
ε'

ε''
0.60 0.03

0.50
0.00
8 10 12 14 16 18
8 10 12 14 16 18
(a) lnω (b) ln ω

Fig. 4  Frequency dependence of a dielectric constant (ε′) and b dielectric loss for Se sample

Se:MWCNTs Se:Graphene
1 kHz 5 kHz 10 kHz 4.00 1 kHz 5 kHz 10 kHz
7.20 50 kHz 100 kHz 500 kHz 50 kHz 100 kHz 500 kHz
1 MHz 1 MHz
6.90
3.80
6.60
ε'
ε'

3.60
6.30

6.00 3.40
300 310 320 330 340 350 290 300 310 320 330 340 350
T (K) T (K)
(a) (b)
Se:MWCNTs Se:Graphene
1.50 1 kHz 5 kHz 10 kHz 0.60 1 kHz 5 kHz 10 kHz
50 kHz 100 kHz 500 kHz 50 kHz 100 kHz 500 kHz
1 MHz 1 MHz
1.20 0.45
0.90
0.30
ε''
ε''

0.60
0.30 0.15

0.00 0.00
290 300 310 320 330 340 350 290 300 310 320 330 340 350
(c) T (K) T (K)
(d)

Fig. 5  Temperature dependence of dielectric constant (ε′) for a Se:MWCNTs, b Se:Graphene samples and dielectric loss, c
Se:MWCNTs, and d Se:Graphene samples

the resistance provided by the surrounding matrix,
the internal temperature of the system must be
raised. Due to the thermal energy, the dipole orienta-
tion starts, thereby, increasing the dielectric constant
as a result. This is an indication of the dipolar-type
dielectric dispersion that is occurring in the present
system [11, 28]. The branched structure of MWCNTs
is also responsible for interfacial polarization, leading
to the increased dielectric constant against tempera-
ture due to the highly conducting nature of MWCNTs
and the positive temperature coefficient effect [29]. The
dielectric loss tangent (tan δ = ε″/ε′) is the ratio of the
dielectric loss (ε″) to the dielectric constant (ε′), for a
dielectric material. The quantity of energy dissipated
in the substance is determined by the dielectric loss,
which is connected with the leakage current (ohmic
conductivity). It occurs when the polarization lags
the applied electric field caused by the grain bound-
ary under an applied A.C. electric field [30]. Stevels
divides the dielectric relaxation phenomenon into
 173 Page 6 of 16 J Mater Sci: Mater Electron (2024) 35:173

three categories: vibrational losses, conduction losses,
and dipole losses. At high temperatures, each of these
losses contributes to dielectric loss. Consequently,
causes dielectric loss to grow as temperature rises [25,
31].
The variation of ε′ and ε″ against frequency at dif-
ferent temperatures is shown in Fig. 6 for thin films
of Se:MWCNT and Se:Graphene. At low frequencies,
both carbon filler composites have a high dielectric
permittivity. It is also asserted that when the frequency
rises, both ε′ and ε″ are reduced rapidly because of
the electrode effect and Maxwell–Wagner interfacial
polarization following Kopp’s theory [32]. The main
cause of the material’s dielectric loss is ion migra-
tion, which attains its peak values at low frequencies
because of contributions from ion jump and ion migra-
tion’s conduction loss [25]. When we impose an elec-
tric field on the nanocomposite film, the dipole and
charge carriers accumulate at the interface between
the conducting nanofillers and the amorphous matrix
[33]. As frequency increases, oscillations of the applied
field increase and corresponding dipolar polarization
characteristics time exceeds the time constant of the
external field and the degree of dielectric polarization
decreases [34]. There is a reduction in ε′ with an
increase in frequency because of the grain boundaries
and decrement in the space charge polarization effect
which depends on the availability of free charge car-
rier and conductivity of the sample [35]. In the lower-
frequency regime, the major contribution of the dielec-
tric dispersion is observed as a result of the dominant
role of the grain boundaries effect that is attributed
to Maxwell–Wagner kind of interfacial polarization
due to significant differences in the conductivity of
the amorphous matrix and the filler [36, 37]. For a
multiphase system, the formation of nanocapacitors
(adjacent conducting MWCNTs surrounded by insu-
lating layers of the amorphous matrix) controls the
interfacial as well as electronic polarization [38]. For
the high-frequency range, both ε′ and ε″ further start
increasing with increasing frequency. When graphene
or CNTs are used as nanofillers in parent selenium to
form the composite materials, they provide a high sur-
face area for effective bonding with the surrounding
matrix material. This reduces the number of interface
states or defects at the filler–matrix interface. Conse-
quently, the number density of the localized charge
traps is also reduced followed by less hindrance to the

Se:MWCNTs
7.2
(a) Se:Graphene
301.3 K 302.5 K 313 K
323.2 K 333.4 K 343.4 K 4.00 (b) 298.1 K 302.6 K
313.1 K 323.4 K
6.8 333.5 K 343.5 K
3.80
ε'

ε'

6.4
3.60

6
3.40
8 10 12 14 16
8 10 12 14 16
lnω lnω
Se:MWCNTs Se:Graphene
1.5
(c) 301.3 K 302.5 K 313 K 0.60 298.1 K 302.6 K
323.2 K 333.4 K 343.4 K (d)
1.2 313.1 K 323.4 K
0.45 333.5 K 343.5 K
0.9
ε''

0.30
ε''

0.6

0.3 0.15

0 0.00
8 10 12 14 16 8 10 12 14 16
lnω lnω

Fig. 6  Frequency dependence of dielectric constant (ε′) for a Se:MWCNTs, b Se:Graphene samples and dielectric loss, c Se:MWCNTs,
and d Se:Graphene samples
J Mater Sci: Mater Electron (2024) 35:173
orientation of dipoles, particularly at higher frequen-
cies. This is probably the reason behind the observed
dielectric behavior of the present samples shown in
Figs. 5 and 6.
According to Rabeya et al., charge carriers move
and assemble at the interface in the presence of an
externally applied field to the composite film because
MWCNTs and gelatin-based polymers have differ-
ent relaxation durations [39]. The large specific area
of MWCNTs provides the enlarged surface area that
is available for interfacial polarization. Leakage cur-
rent increases the dielectric loss due to variations in
the positive and negative space charge distributions
caused by surface lattice defects and interfaces [40,
41]. Dwivedi et al. examined the dielectric behavior
of CNTs-incorporated ­Cu5Se75Te10In10 glasses and
observed the rise in dielectric parameters with the
increasing concentration of CNT [42]. The enhanced
dielectric constant (142.1) and dielectric loss (3665.5)
were reported by Khan et al. over the incorporation
of 5-wt % MWCNTs in the host ­Ga10Se10 system with
the dielectric constant and dielectric loss of 36.31 and
34.08, respectively [43]. The relaxation process associ-
ated with the friction against dipole motion dropping
with frequency may be indicated by the increase in
dielectric constant with frequency.
3.2 S
 tudy of thermally activated A.C.
conduction
The material’s electrical conductivity shows the
extent of response or transfer of free charge carri-
ers present in a material when we apply an external
electric field. The electrical A.C. conductivity (σac)
obeys a power law known as the “Universal dielectric
Se:MWCNTs
-12
(a) 301.3 K 302.5 K
313 K 323.2 K
333.4 K 343.4 K
-15
lnσac
-18
-21
-24
8 10 12 14
lnω
Fig. 7  Measured A.C. conductivity (lnσac) for a Se:MWCNT and b Se:Graphene samples as a function of frequency (lnω) at different
temperatures
Page 7 of 16 173
response (UDR) model,” which is indicated by a linear
dependence with frequency in the ln σac versus ln ω
plot. According to the UDR model, the σac is the sum
of a constant (resistive), and a frequency-dependent
(capacitive) factor in which material can be treated
with an analogous R–C electric circuit. The electrical
conductivity of a sample is represented by [44] with
frequency-dependent alternating current caused by
the out-of-phase movement of charges
𝜎ac (w) = 𝜎(0) + AwS (1)
where s is the power-law exponent which measures
electrical conduction and relaxation behavior and
indicates how strongly charge carriers and polarons
interact with their surroundings; s is also found to be
temperature dependent [45].
The distributions of the electric field in the system
and the disturbances caused by the electric field are
well understood by the electrical A.C. conductivity
measurements. The variation of A.C. conductivity as
a function of frequency and temperature is shown in
Figs. 7 and 8. The hopping process, which is brought
about by the application of the electric field, is thought
to be the cause of the conductivity increases with fre-
quency. From Fig. 7, we can conclude that the A.C.
conductivity increases with increasing frequency in
a temperature span of 290–350 K. In a high-frequency
regime, A. C. conductivity shows a weak temperature
dependence. The development of conductive channels,
which aid in current transfer, can be used to explain
the increase in conductivity. Since the 1D geometry of
CNTs is better suited for the development of conduc-
tive frameworks than the 2D shape of graphene sheets,
doping of MWCNTs permits more favorable condi-
tions than the addition of graphene sheets [46, 47]. As
Se:Graphene
-10
298.1 K 302.6 K
(b) 313.1 K 323.4 K
-13 333.5 K 343.5 K
-16
lnσac
-19
-22
-25
16 8 10 12 14 16
lnω
 173 Page 8 of 16 J Mater Sci: Mater Electron (2024) 35:173

Se:Graphene
Se:MWCNTs
-12 1 kHz 5 kHz 10 kHz
1 kHz 5 kHz 10 kHz
-12 50 kHz 100 kHz 500 kHz
(b) 50 kHz 100 kHz 500 kHz
(a) 1 MHz 1 MHz
-15
-15

lnσac
-18
lnσac

-18
-21
-21

-24 -24
2.80 3.00 3.20 3.40 2.80 3.00 3.20 3.40

1000/T (K-1) 1000/T (K-1)

Fig. 8  Variation of A.C. conductivity (lnσac) for a Se:MWCNT and b Se:Graphene samples as a function of inverse of temperature at
specific frequencies

a result, Se:MWCNTs thin film has a greater conduc-
tivity than Se:Graphene thin film for the same filler
concentration because each CNT exhibits extremely
small contact resistance [46, 47]. Bao et al. proposed a
contact resistance model to explain the electrical con-
ductivity of carbon nanotube nanocomposites based
on the electron transport theory [48]. The chirality and
diameter of the CNTs’ walls determine the energy
bands that contribute to conduction, and the contact
resistance between two CNTs is generated by the bal-
listic movement of electrons along tunneling channels
[49]. The relationship between logarithmic A.C. con-
ductivity (i.e., log σac) and the inverse of absolute tem-
perature (i.e., 1/T) is depicted in Fig. 8. In the present
coated thin-film samples, the particular thermally gen-
erated conduction was abandoned. The exponential
variation of A.C. conductivity with the temperature in
the low-frequency region is responsible for such tem-
perature dependence, while it exhibits temperature-
independent behavior in the high-frequency zone.
The relationship between electrical conductivity and
temperature predicts a thermally activated electron
hopping conduction behavior [50]. Various models
such as the quantum–mechanical tunneling model
(QMT), [51] non-overlapping small polaron tunneling
model (NSPT), [52, 53] overlapping large polaron tun-
neling model (OLPT), [54] and correlated barrier hop-
ping (CBH) model [25, 32, 45] were proposed by many
scientists to understand relaxation dynamics caused
by the hopping or tunneling of electrons to explain the
A. C. conduction mechanism.
The measured A.C. conductivity data are fitted
with the least square straight line using Eq. (1) which
yields the frequency exponent (s) values. The varia-
tions of power-law exponent (s) with temperature are
shown in Fig. 9a and b, respectively, for Se:MWCNTs
and Se:Graphene nanocomposites. The temperature
dependence of power-law exponent “s” with tempera-
ture shown in Fig. 9a reveals that the correlated barrier
hopping (CBH) model is the conduction mechanism
that causes the frequency exponent s for Se:MWCNTs
nanocomposite thin film to drop as temperature

Se:MWCNTs Se:Graphene
0.90 (a) 0.70 (b)

0.85 0.65

0.80 0.60
S

0.75 0.55

0.70 0.50
300 310 320 330 340 350 290 300 310 320 330 340 350
T(K) T(K)

Fig. 9  Variation of power-law exponent (s) with temperature for a Se:MWCNT and b Se:Graphene samples as a function of temperature
J Mater Sci: Mater Electron (2024) 35:173 Page 9 of 16 173

increases [see, 25, 32, 45]. However, the increasing hopping is anticipated to be the major conduction
nature of s with rising temperature shows that the mechanism for Se:MWCNTs.
Non-overlapping Small Polaron Tunneling (NSPT) On the other hand, the nature of variation of s
model is the most appropriate conduction mechanism with temperature for Se:Graphene indicates NSPT
for thin film of Se:Graphene nanocomposite [see 45, conduction mechanism. Due to trapped charge car-
53, 54]. riers or polarons tunneling across grain boundaries
Elliott explains the conduction mechanism in amor- or structural flaws in the current Se:Graphene nano-
phous solids and the proposed model explains the role composite, this kind of A.C. conduction is possibly
of the temperature dependence of A.C. conductivity expected. If the inclusion of a charge carrier to a loca-
[55]. According to the CBH model, the power-law tion results in such severe localized lattice distor-
exponent (s) is expressed as follows [56]: tion that the system’s overall energy is reduced by
a portion of the polaron energy WH, a tiny polaron
may arise in a covalent solid [58] according to the
6KB T
S=1− ( ) (2)
WM + KB Tln 𝜔𝜏0 NSPT model. For this model the A.C. conductivity
is expressed as follows:
In Eq. (2), τ0 denotes the characteristic relaxation
time, while the height of the energy barrier of dif- [ ( )]2
e2 𝜋 4 KB T N EF 𝜔R𝜔 4
fusion or hopping path is represented by WM. The 𝜎ac = (5)
evaluated values of WM are presented in Table 1. The
24𝛼
potential barrier between the two charged defect In Eq. (5), the inverse of α denotes the localization
states, ­D+ and ­D-, will be concurrently crossed by length of small polarons corresponding to their wave
two polarons in the CBH model, and the height of the function. The power-law exponent (s) for the NSPT
barrier is connected with the interstice distance via a model is given by
Coulombic interaction [57]. The A.C. conductivity can
be represented as the following using the CBH model:
4
S=1−
(6)
( ) ( )
1 W
[ ( )]2 ln 𝜔𝜏 − K HT
H B
n𝜋 3 e2 N EF 𝜀𝜀0 𝜔R𝜔 6
𝜎ac = (3)
24 Here, τH is Debye relaxation time and WH is the
polaron hopping energy. For the NSPT model, the
where N(EF) is the density of defect states, n is the hopping distance Rω, can be written as follows:
number of polarons involved in the hopping process,
and ε is the dielectric constant. The polaron hopping
[ ( ) ]
WH
(7)
1 1
R𝜔 = −
distance Rω at a specific value of ω can be expressed
ln
2𝛼 𝜔𝜏H KB T
as follows:
The values of different parameters of the NSPT
ne2 model for Se:Graphene nanocomposite are tabulated
R𝜔 = (4)
in Table 2.
[ ( )]
𝜋𝜀𝜀0 WM + KB Tln 𝜔𝜏0

The calculated values of R ω and N(E F) are tab-

ulated in Table 1 for Se:MWCNTs. The bipolar

Table 1  A.C. conductivity (σac) data and power-law exponent (s) Table 2  A.C. conductivity (σac) data and power-law exponent (s)
fitted parameters from CBH model of Se:MWCNTs nanocom- fitted parameters from NSPT model of Se:Graphene nanocom-
posite at 302.5 K posite at 302.6 K
f (kHz) ε′ ε″ WM (eV) Rω (Å) N(EF) f (kHz) ε′ ε″ WH (eV) Rω (Å) N(EF)
(× ­1021 ­eV−1 ­cm−3) (× ­1028 ­eV−1 ­cm−3)

1 6.37 0.15 1.83 6.79 4.17 1 3.74 0.34 0.26 44.04 5.63
10 6.28 0.06 1.76 6.88 2.64 10 3.52 0.11 0.20 43.87 3.24
100 6.24 0.11 1.70 6.92 3.38 100 3.46 0.06 0.14 43.70 2.27
 173 Page 10 of 16 J Mater Sci: Mater Electron (2024) 35:173

3.3 Observation of Meyer–Neldel rule the Meyer–Neldel empirical rule and the term EMN
is known as Meyer–Neldel energy [62]. The MNR is
The thermally activated A.C. conduction in amorphous applicable for several types of substances, especially
semiconductors can be studied in terms of the following chalcogenide glasses [63], and organic semiconduc-
relation [59]: tors [64] The shifting of the fermi level shift with tem-
( ) perature and an exponential distribution of density
ΔEc
𝜎ac = 𝜎0 exp − (8) of states (DOS) have been suggested as the cause of
kB T the MN rule in inorganic amorphous semiconductors
[65, 66]. The Meyer–Neldel energy is said to be closely
As it is clear from the equation above, the slope of
correlated with the width of the density of states in
semi-logarithmic graphs of the σac against the inverse
the disordered energy band, according to theoretical
of absolute temperature can be used to calculate the
research by Fishchuk et al. [64].
A.C. conduction energy (Ec). From Fig. 10a one can
Following the reverse MNR of the electronic trans-
see that ∆Ec decreases with increasing frequency for
port mechanism of the thin film of Se:MWCNTs, we
Se:MWCNTs nanocomposite thin film, while the reverse
have seen a negative connection between the expo-
trend is observed for Se:Graphene nanocomposite film
nential pre-factor (σ00) and activation energy (ΔE)
in Fig. 10b. The increase in applied frequency, which
(see Fig. 11a), which is noticeably different from the
boosts the electrical jump between localized states and
normal trend. The thin film of Se:Graphene follows
confirms that hopping conduction is the predominant
the MNR in the hole transport phenomena as shown
mechanism, may be responsible for this drop [60].
in Fig. 11b. The values of characteristic energy EMN
The estimated values of activation energies for the
and pre-exponential factor σ00 are 16.7 meV, 1.25 × ­10–5
Se:MWCNTs nanocomposite thin film are in the range
(Ω cm)−1, and 14.9 meV, 4.49 × 1­ 0–12 (Ω cm)−1 for thin
of 35–98 meV, while for the studied Se:Graphene sample
films of Se:MWCNTs and Se:Graphene, respectively.
the activation energy lies between 135.8 and 164.3 meV.
To explain the cause of reverse MNR occurrences,
When a phenomenon [61] is governed by thermally acti-
Lucovsky et al. suggested a statistical shift model [67]
vated physical, chemical, and physicochemical quanti-
that depends on the band orientation of the various
ties, then it follows the Arrhenius relation given by
phases of nanocrystalline grains distributed across
Eq. (8). The experimental results suggest the following
an amorphous matrix. A reverse MNR with negative
correlation of activation energy of a thermally triggered
MN characteristic energy (EMN) reflects the shifting
A.C. conduction with the corresponding pre-factors:
of fermi energy into the band tail states of the sur-
rounding disordered amorphous regions [68]. The fre-
( )
ΔE
𝜎0 = 𝜎00 exp (9) quency dependence of dielectric loss is explained by
EMN
Giuntini [69] by considering the hopping model over a
Equation (9) gives the dependence of pre-factor potential barrier between localized sites in which each
𝜎0 on the activation energy (∆E) and is known as pair of disordered sites forms a dipole to explain the

0.120 0.170
Se:MWCNTs (b) Se:Graphene
(a)
0.160
0.090
∆E (eV)
∆E (eV)

0.150

0.060
0.140

0.030 0.130
0 500 1000 1500 0 5 10 15
f (kHz) f (kHz)

Fig. 10  Variation of A.C. conduction energy (∆E) with frequency for a Se:MWCNT and b Se:Graphene samples
J Mater Sci: Mater Electron (2024) 35:173 Page 11 of 16 173

Se:MWCNTs Se:Graphene
-13 -14.5
(a) (b)
-13.5 -15
EMN = 14.86 meV
-14 R² = 0.9776 -15.5 σ00 = 4.49 × 10-12 (Ω-cm)-1
lnσ0

lnσ0
-14.5 EMN = 16.67 meV -16
σ00 = 1.25 × 10-5 (Ω-cm)-1 R² = 0.9967
-15 -16.5
-15.5 -17
0.030 0.040 0.050 0.060 0.070 0.135 0.145 0.155 0.165
∆E (eV) ∆E (eV)

Fig. 11  Meyer–Neldel plot for A.C. conduction in as-prepared a Se:MWCNT and b Se:Graphene samples

dielectric dispersion in a particular temperature and/ for lower-frequency range. To prevent their distortion
or frequency region. Then, we can combine the dielec- clouds from overlapping, it is assumed that the small
tric loss with the circular frequency ω of the applied polarons are localized. At low temperatures, they
field, as follows: behave as free particles with enhanced mass, while at
high temperatures, they move by thermally activated
hopping [58]. The activation energy for polaron trans-
3
ne2
𝜀�� (w) = 𝜀o − 𝜀∞ 2𝜋 2 N( ) KB T𝜏o m WM −4 wm (10)
( )
𝜀0 fer (WM/WH), hopping /tunneling distance (Rω), and
the density of defect states at Fermi level [N(EF)] is
Here, n and N are the numbers of hopping elec-
deduced from the fitted curves using the expressions
trons and the number density of localized sites,
given in (CBH and NSPT) conduction mechanisms for
respectively. The value of Wm also referred to as the
both the samples. Figure 13a and b show the varia-
binding energy of charge carriers in localized states,
tion of temperature-dependent activation energy for
is the energy needed to transfer an electron from one
polaron transfer for Se:MWCNTs and Se:Graphene
site to infinity [55, 70]. In Fig. 12, we have plotted the
samples, respectively. The lowering character of WM
variation of ln ε″ against ln ω at various temperatures
with rising temperature may be related to an increase
and from the figure, we can conclude that the disper-
in the degree of overlapping potential wells in the
sion loss increases for the high-frequency regime in
closest surrounding sites. Since the thermal activa-
MWCNTs-doped nanocomposite, while a reverse
tion energy overlaps the potential well linked with the
trend is observed for graphene-doped nanocomposite
nearby sites in the Pike theory of electron transmission

Se:MWCNTs Se:Graphene
0.5 301.3 K 302.5 K 313 K
(a) -0.5 298.1 K 302.6 K 313.1 K
0.0
323.2 K 333.4 K 343.4 K (b)
323.4 K 333.5 K 343.5 K
-1
-0.5
-1.5
-1.0
lnε''

lnε''

-1.5 -2

-2.0 -2.5

-2.5 -3
-3.0
13.0 14.0 15.0 16.0 -3.5
8 9 10 11 12 13
lnω
lnω

Fig. 12  Variation of lnε″ against lnω for as-prepared a Se:MWCNT and b Se:Graphene samples
 173 Page 12 of 16 J Mater Sci: Mater Electron (2024) 35:173

[55, 71, 72]. Figure 14a and b shows the variation of the for the bulk samples as compared to that of the thin-
hopping/tunneling distance Rω as a function of tem- film samples. The effect of the interfacial layer is more
perature at different frequencies of (a) Se:MWCNTs pronounced for the thin-film samples due to the small
and (b) Se:Graphene samples. The figure shows that, grain size. This low dielectric constant interfacial layer
as the temperature rises, the thermal energy of the acts as a series capacitor with the present thin-film
polarons increases. Due to the increased inter-chain samples and therefore decreases the overall values
interaction (electric charge jump), the hopping dis- of ε′ and ε″. Similar results have been reported by
tance increases with temperature [58]. The calcu- other research groups [75, 76]. As a disordered semi-
lated values of density of defect states near the Fermi conductor, amorphous selenium primarily transports
level [N(EF)] are summarized in Table 1 and 2 for charges through the hopping of electrons. The crea-
Se:MWCNTs and Se:Graphene samples, respectively. tion of small conductive islands and hopping in the
According to Jana et al., the assessed values of [N(EF)] amorphous matrix together with conducting fillers
indicate that the primary charge transfer mechanism like MWCNTs and graphene contribute to the overall
is charge carrier hopping, which takes place between conductivity. Further, the dielectric nature of selenium
the closest nearby sites [71]. and the conductive nature of MWCNTs and graphene
Analysis of the dielectric constant and loss for the fillers helped in composing micro-capacitors inside
current Se:MWCNTs and Se:Graphene samples in the amorphous polymeric matrix of the host element
comparison to their bulk equivalents [73, 74] is tabu- Selenium as shown in Fig. 15.
lated in Table 3. A thorough inspection of this table
reveals that the values of both ε′ and ε″ are higher

Se:MWCNTs Se:Graphene
0.30 (b) 1 kHz 10 kHz 100 kHz 1 MHz
2.00 (a) 1 kHz 10 kHz 100 kHz 1 MHz

0.23
1.70
WH (eV)
WM (eV)

1.40 0.15

1.10 0.08

0.80 0.00
290 300 310 320 330 340 350 300 310 320 330 340 350
T(K) T (K)

Fig. 13  Variation of temperature-dependent activation energy for polaron transfer of a Se:MWCNT and b Se:Graphene samples

Se:MWCNTs Se:Graphene
14 1 kHz 10 kHz 100 kHz 1 MHz 52
(a) (b) 1 kHz 10 kHz 100 kHz 1 MHz
50
12
R ω (Å)

48
R ω (Å)

10
46
8
44
6 42
300 310 320 330 340 350 300 310 320 330 340 350
T(K) T (K)

Fig. 14  The variation of the tunneling distance Rω as a function of temperature at different frequencies of a Se:MWCNT and b Se: Gra-
phene samples
J Mater Sci: Mater Electron (2024) 35:173 Page 13 of 16 173

Table 3  Comparison of
f (kHz) Se:MWCNTs Se:Graphene
dielectric constant and
dielectric loss for bulk and Bulk Thin film Bulk Thin film
thin-film samples at room ε′ ε″ ε′ ε″ ε′ ε″ ε′ ε″
temperature [73, 74]
1 60.29 1.34 × ­105 6.37 0.15 122.84 1.15 × ­106 3.74 0.34
10 48.01 1.29 × ­104 6.28 0.07 132.04 1.03 × ­105 3.52 0.11
100 45.42 1.16 × ­103 6.24 0.11 121.46 1.02 × ­104 3.46 0.06

Fig. 15  Formation of micro-capacitors inside the amorphous polymeric matrix of the host element Selenium due to conducting a gra-
phene fillers and b MWCNTs fillers

4 Conclusion Author contributions

The dispersion behavior of A.C. conductivity in thin-
film samples is found to be consistent with Jonscher’s
universal power law. The Meyer–Neldel correlation
is observed between the pre-factors and activation
energies for the A.C. conductivity data of present
Se:MWCNTs and Se:Graphene samples. The research
outcome of dielectric constant and loss indicates that
CNTs and functionalized graphene sheets make excel-
lent nanofillers for creating novel polymer composites
with high dielectric constant values. In addition, the
conductive nature of MWCNTs and graphene fillers
contributes to the construction of micro-capacitors
inside the amorphous polymeric matrix of the host
element Selenium.
SKY contributed to Writing and Original draft prepa-
ration, Methodology, and Software. SSF and HEA
contributed to Thin-film preparation and Electrical
characterization. NM contributed to Conceptualiza-
tion, Writing a final draft, and Reviewing and Editing
of the manuscript.
Funding
This work is supported by the IoE scheme (Dev.
Scheme No. 6031) and CSIR, New Delhi, (Scheme No.
03(1453)/19/EMR-II) to Neeraj Mehta.

Data availability
Acknowledgements
The data underlying this article are available in the
Neeraj Mehta acknowledges his university for pro- article. The datasets generated during and/or analyzed
viding an incentive grant under the IoE scheme (Dev. during the current study are available from the cor-
Scheme No. 6031). He is thankful to CSIR, New Delhi, responding author upon reasonable request.
India for providing financial support under a Project
(Scheme no. 03(1453)/19/EMR-II). Sachin Kumar Yadav
is grateful to CSIR, New Delhi, India for providing a
junior research fellowship under the same Project.
 173 Page 14 of 16
Declarations
Conflict of interest The authors certify that there is
no conflict of interest.
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