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 Journal of Physics D: Applied Physics

J. Phys. D: Appl. Phys. 54 (2021) 295104 (7pp) https://doi.org/10.1088/1361-6463/abfbfa

Determination of interlayer electron

mobility in multilayer MoS2 flake using
impedance spectroscopy
Shikha Srivastava1 and Yashowanta N Mohapatra1,2,3,∗
1
Materials Science Programme, Indian Institute of Technology Kanpur, Kanpur 208016, India
2
Department of Physics, Indian Institute of Technology Kanpur, Kanpur 208016, India
3
National Centre for Flexible Electronics, Indian Institute of Technology Kanpur, Kanpur 208016, India

E-mail: ynm@iitk.ac.in

Received 5 January 2021, revised 14 April 2021

Accepted for publication 27 April 2021
Published 14 May 2021

Abstract
Layered molybdenum disulfide (MoS2 ) is emerging as a promising candidate for novel
electronic applications, though the focus has largely been on few-layered thin films and in-layer
electrical properties. MoS2 shows various nontrivial departures in its electrical properties in
comparison to isotropic crystalline materials, however the understanding of anisotropic
properties, particularly of charge carrier mobility in MoS2 flakes, is meagre. We experimentally
study inter-layer mobility in mechanically exfoliated MoS2 flakes. The choice of a suitable
sandwich device structure enables us to study the inter-layer transport using temperature
dependent current–voltage (J–V) and impedance spectroscopy. The separation of peaks in the
imaginary part of impedance i.e. Im (Z) spectra due to defects and transport in the space charge
limited regime allows measurement of mobility un-encumbered by other effects. We study
flakes obtained from both naturally occurring and synthetic crystals. The calculated inter-layer
mobility (µ⊥ ) exhibits µ⊥ ∼ Tδ temperature dependence with δ = 1.6 and thereby revealing
that impurity scattering is the dominant mechanism. A further confirmation that the mobility is
limited by charged impurity scattering comes from the observation that it improves for
temperatures lower than a characteristic temperature, which marks deionization of donor
impurities. Our results provide a direct estimation of the inter-layer mobility in exfoliated MoS2
flakes and would lead to carrier transport engineering and design strategies for applications
based on MoS2 flakes.

Supplementary material for this article is available online

Keywords: MoS2 , mobility, impedance spectroscopy, TMDC

(Some figures may appear in colour only in the online journal)

1. Introduction [1–6]. Molybdenum disulfide (MoS2 ) is the most abundant

Since the realization of two dimensional layer of graphene,
immense efforts have been invested in exploring the family of
layered transition metal dichalcogenides (TMDC) because of
their fascinating electrical, optical and mechanical properties
∗
Author to whom any correspondence should be addressed.
TMDC compound and is being envisioned as future material
due to their possible uses in flexible electronics, solar energy
harvesting devices and next generation electronic and opto-
electronic applications [7–14]. MoS2 crystallizes in two poly-
types; rhombohedral (3 R) and hexagonal (2 H), but naturally
occurring MoS2 crystals are predominately of 2 H type and
show semiconducting properties [15, 16]. MoS2 crystals con-
sist of stacks of large number of atomic layers in which atoms

1361-6463/21/295104+7$33.00 1 © 2021 IOP Publishing Ltd Printed in the UK

J. Phys. D: Appl. Phys. 54 (2021) 295104
of sulfur and molybdenum (S–Mo–S) are bonded together
by strong covalent bonding, whereas layers are held together
by weak inter-layer interaction. Presence of weak inter-layer
bonding facilitates the exfoliation of MoS2 crystal in stable
monolayer and multilayer flakes which shows remarkably dif-
ferent electrical and optical properties [17–19]. It has been
reported that in comparison to monolayer, multilayer MoS2
(m-MoS2 ) flake has relatively high dielectric constant and can
sustain high electrical power [20]. Moreover, the presence of
an indirect bandgap (1.2 eV) comparable to silicon (Si) offers a
wide spectral response. Thus m-MoS2 flakes could be thought
of as an important complement to silicon. Recently, multilayer
MoS2 has been embedded in various devices, including FETs,
sensors, and phototransistors, but the electrical properties of
such m-MoS2 are not well explored [8, 20–24]. Therefore, to
harness full potential of the m-MoS2 flake, a systematic study
of its electrical properties is desired. Some recent reports men-
tioned anisotropic behaviour of layered TMDC and showed
that MoS2 exhibits highly anisotropic electronic and mechan-
ical properties in comparison to isotropic crystalline materials
such as Si and Ge [18, 25, 26]. For instance, dielectric con-
stant in MoS2 is highly direction dependent and profoundly
depends on the number of layers present in the stack of the
m-MoS2 [27, 28]. Carrier mobility and lifetime are the key
material parameters, and are known to be highly dependent
on local dielectric environment; this evidently inspires the
investigation of anisotropy in the mobility of m-MoS2 . Nearly
five decades ago, the first comprehensive study of charge car-
rier mobility in MoS2 single crystal was carried out by Fivaz
and Mooser, in which the room temperature Hall mobility of
charge carrier in m-MoS2 was found to be in the range 200–
500 cm2 V−1 s −1 with phonon scattering as the dominant
mechanism above 200 K [29, 30]. In a more recent report Das
et al observed that the carrier mobility is highly dependent
on the thickness of MoS2 flake [31]. However, these mobility
estimations utilize FET architecture and multi-terminal Hall
measurements. Generally, in these techniques, device config-
uration, as well as contact resistance plays a very crucial role
in mobility estimation [32, 33]. In contrast, we observe that
impedance spectroscopy tracks the time constant associated
with different relaxation processes occurring in material and
thus offers the most reliable estimate of charge carrier mobility
in comparison to other popular techniques of mobility meas-
urements, and is especially suited for inter-layer studies with
simple device structure [34, 35].
In this work, we measure inter-layer mobility (µ⊥ ) of mech-
anically exfoliated MoS2 flakes. For this purpose, we util-
ize the most straight forward device structure consisting of
a thick m-MoS2 flake sandwiched between two electrodes to
obtain suitable current density voltage (J–V) characteristics.
The mobility is measured using the analysis of complex part of
impedance spectra (Im (Z)) in impedance spectroscopy [34].
We study flakes obtained from both synthetic and nat-
urally occurring crystals for comparison. The natural MoS2
single crystals are geological crystals and usually obtained
from the crystallization of mineral molybenite. Since, these
natural crystals are directly taken out of the mines therefore
has a possibility of possessing large amount of impurities. In
2
S Srivastava and Y N Mohapatra
most instances, synthetic single crystals are grown in more
controlled environment by chemical vapor deposition using
various carrier gases. Thereby the synthetic single crystals are
generally of higher grade compared to natural crystals in terms
of purity and defect concentration. The reported carrier density
for bulk MoS2 is in range ∼1015–16 cm−3 [36, 37].
The structure and naming of the two types of devices are as
follows:
I-a-N: Au|m-MoS2 flake (natural)|ZnO
I-b-S: Au|m-MoS2 flake (synthetic)|ZnO
A detailed temperature dependent J–V characteristics and
impedance spectroscopy were carried out to characterize these
devices. We utilize complex part of the impedance spectra
Im (Z) in the space charge limited current (SCLC) regime to
determine the inter-layer charge carrier mobility. Our results
provide an insight into the direction dependent charge car-
rier transport, and this approach would further lead to tailor
and design the multilayer MoS2 based electronic devices for
optimum performance. It is to be noted that the proposed
method is generic and can be suitably applied to measure fun-
damental charge transport properties in all layered materials.
2. Experimental details
The schematic of the fabricated Au|m-MoS2 |ZnO device is
presented in figure 1(a). For the fabrication of devices we
utilize commercially available natural and synthetic MoS2
(n-type) single crystals. We performed standard mechanical
exfoliation process to obtain a flake of thickness ∼10 µm. The
exfoliated flakes were thoroughly cleaned using acetone and
IPA solution to remove contamination and traces of adhesive
materials. After cleaning, flakes were examined under optical
microscope to identify smooth region (free from mechanical
damages) for the deposition of metal electrodes as shown
in inset of figure 1(b). After this identification, MoS2 flakes
were sandwitched between two shadow masks. Further, MoS2
flakes along with shadow masks were transferred for vacuum
deposition of the electrodes. These shadow masks have cir-
cular opening of 1 mm diameter to leave space for the bot-
tom and top electrodes. On one side of each m-MoS2 flake,
a 100 nm thick ZnO:Al (2 wt% aluminum doped) film was
deposited using pulsed DC magnetron sputtering technique.
After ZnO:Al deposition, flakes along with mask are trans-
ferred in thermal evaporator chamber to deposit gold (Au)
electrode of thickness 100 nm. The Au contact acts as the
bottom ohmic electrode. After the electrode deposition, each
m-MoS2 flake was carefully removed from shadow masks
and mounted on a TO-header using conductive silver paste.
Electrical connections to outer pins of TO-header were made
using Au wire of thickness 25 µm. Finally, to avoid any
mechanical damage, the device is sealed with a metal cap
on TO-header, as shown in figure 1(c). Temperature depend-
ent J–V characteristics of the fabricated device were conduc-
ted utilizing Keithley-2601 Source Meter Unit, which has the
noise limit in 100 pA for applied voltages up to 40 V. The
Im (Z) characterizations of the device were measured using
Agilent Impedance 4294 A precision impedance analyzer.
J. Phys. D: Appl. Phys. 54 (2021) 295104
Figure 1. Schematic representation and fabricated device. (a) Schematic of the Au|m-MoS2 |ZnO device. (b) Optical microscopy image of
the exfoliated m-MoS2 flake. Inset depicting flat area of the flake used for device fabrication. (c) Picture of the fabricated device capped
inside TO header.
These measurement setups were connected to He-gas based
closed cycle refrigerator incorporated with the Lakeshore
temperature controller to perform the measurements in the
temperature range 8 K–300 K.
3. Result and discussion
The device structures are chosen such that they form single
carrier diodes to enable characterization using J–V character-
istics and impedance spectroscopy. The electron affinity of the
m-MoS2 is 4 eV, whereas the work function of Au and ZnO
are 5.1 eV and 4.7 eV, respectively [38, 39].
Therefore, it forms a built-in potential (V bi ) at the
m-MoS2 |ZnO interface. Since ZnO acquires an accumulation
region and depletion region is formed in m-MoS2, thereby res-
ulting in a barrier at the m-MoS2 |ZnO interface to the inject-
ing electrons. It is known that Au acts as an ohmic contact to
MoS2 . In our fabricated Au|MoS2 |Au device the ohmic nature
of Au is further verified by the linear J–V characteristics as
shown in figure S1 (available online at stacks.iop.org/JPD/
54/295104/mmedia), in section 1 of supplementary material
[40–42].
Therefore, the transport properties in these devices are
mainly controlled by the interface quality and the barrier
at the MoS2 |ZnO interface. Figures 2(a) and (b) depict the
semi-log plot of J–V characteristics for the devices I-a-N
3
S Srivastava and Y N Mohapatra
and I-b-S, respectively. The J–V characteristics were meas-
ured at a temperature ranging from 8 K–300 K. As shown in
figure 2(a), I-a-N device possesses weak rectifying behaviour.
However, the J–V characteristic of the I-b-S device exhibits
excellent rectifying behaviour over the entire measured tem-
perature range. In I-b-S device, under the forward bias, elec-
trons can easily flow from MoS2 to ZnO due to the lowering
of the barrier seen by the electrons. On the other hand, an
effective Schottky barrier suppresses the flow of charge car-
riers in reverse bias. This results in the rectification of the
order 103 . However, in I-a-N device, poor rectifying beha-
viour possibly arises from the large amount of impurity con-
centration that allows the charge carriers to readily flow in
both directions on applying forward and reverse bias. The
J–V characteristics of both the devices I-a-N and I-b-S are re-
plotted in the log-log scale, as shown in section 2 of the sup-
plementary material. The J–V characteristics of the devices
measured at different temperatures (8 K to 300 K) follow
power-law voltage dependence (J α V n ). At low bias, slope
n ∼ 1 was observed indicating that the charge conduction is
ohmic in nature. Whereas, at higher voltages, n deviates from
1 (n > 2) suggests trap limited SCLC implies the trap filling
in bulk
One striking feature is that the reduction in absolute values
of the current is not monotonic with temperature.
As shown in figure 2, for both devices I-a-N and I-b-S,
the current density shows its minimum value and looks more
J. Phys. D: Appl. Phys. 54 (2021) 295104 S Srivastava and Y N Mohapatra

Figure 2. Temperature dependent J–V characteristics. J–V

characteristics of Au|m-MoS2 |ZnO device with (a) natural m-MoS2
(I-a-N) flake and (b) synthetic m-MoS2 (I-b-S) flake, measured in
the temperature range 18.5 K to 297.1 K.

exponential with voltage at around 37 K (indicated by arrow),

at this temperature the charge carrier concentration is suddenly
reduced due to carrier freeze out, ostensibly due to Fermi level
crossing the donor level in the gap.
For the estimation of mobility, impedance measurements
were carried out in the SCLC regime. A typical set of imped-
ance spectra for both the fabricated devices I-a-N and I-b-S
is recorded as a function of temperature. The characteristic
frequencies for specific charge carrier relaxation mechanisms
appear as peaks in such plots. In brief the principle of mobil-
ity measurement is based on the fact that in the SCLC regime,
the peak in Im (Z) appears when the reciprocal of the transit
time of the charge carrier across the device matches the fre-
quency of the probing signal. Though defects charging and
discharging can also lead to such a peak, in practice it is not
difficult to distinguish between the two. The variation of Im
(Z) versus frequency recorded at 2 V (i.e. at V > V bi ) for tem-
perature range 8 K–300 K, as shown in figure 3. Both plots
show the typical decrease of impedance as the temperature
Figure 3. Temperature dependent Im (Z) versus frequency
characteristics of Au|m-MoS2 |ZnO device with (a) natural m-MoS2
(I-a-N) flake and (b) synthetic m-MoS2 (I-b-S) flake, measured in
the temperature range 17.7 K to 298.1 K. The continuous lines are
fitted to the simulation of lumped circuit model as shown in (c).
increases except at and below 37 K. The I-a-N device exhibits
two well separated Im (Z) peaks, whereas two closely spaced
Im (Z) peaks are observed for the I-b-S device. The frequency
dependence of impedance and the time constants associated
with these peaks are analyzed. In I-a-N device, the time con-
stant corresponding to low frequency peaks (at 10 kHz fre-
quency) seems to be weakly temperature dependent. To get

4
J. Phys. D: Appl. Phys. 54 (2021) 295104 S Srivastava and Y N Mohapatra

more insight, normalized Im (Z) is plotted against frequency

(see section 3 of supplementary material) which clearly shows
that the apparent temperature-shift in time constant is observed
because of superposition of two components of time constants
with the slower component of time constant dominating at low
temperature, and the faster component dominating at higher
temperature. Thus, the charge processes occurring at mid gap
defect states are responsible for the appearance of the peaks in
low frequency regime. The time constant associated with the
process is moderately temperature independent. Since the trap-
ping and de-trapping of charge carriers in the trap states show
temperature dependent time constants, therefore, defect states
in our fabricated device acts as generation-recombination (g-r)
centers. These g-r centers have the capability of capturing or
emitting charge carriers and hence deteriorate the performance
of the device.
However, the peak in Im (Z) plot at high frequency regime
is due to the charge carrier transport as has been shown earlier
and characteristic time constants associated with these peaks
provide the information of the mobility of charge carriers [34].
For the I-b-S device, Im (Z) vs frequency plot exhibits two
overlapping peaks. However, only transport related peak at
the higher frequency is monitored for mobility extraction. The
experimental Im (Z) data is fitted with equivalent circuit rep-
resented by two standard RC networks connected in series and
is given by the formula
1 1
Z = Rs + + (1)
1
+ jωC1 1
+ jωC2
R1 R2
where Rs is the series resistance, R1 , R2 and C1 , C2 are the res-
istances and capacitances corresponding to bulk and interface,
respectively. Here, ω represents the monitoring frequency.
The steady state charge carrier mobility can be expressed as
d2
µ= (2)
τdc (V − Vbi )
where d is the thickness of m-MoS2 flake, V is the applied
voltage, Vbi represents the built-in voltage, and τdc is the dc
carrier transit time. The dc carrier transit time is related to
the ac transit time (τp ) by the expression τdc = κτp , where
κ = 0.56, is a numerical factor for dispersive and non-
dispersive transports [43].
Using the expression (2), electron mobility has been extrac-
ted for both I-a-N and I-b-S devices. The extracted temperat-
ure dependent mobility is plotted in figure 4, which depicts
that the mobility follows power-law temperature dependence
above T > 37 K and varies as µ ≈ Tδ . Here, δ is the power expo-
nent, which depends on carrier density, temperature, and dom-
inant scattering mechanism. By fitting the calculated mobility
with a three parameter polynomial function µ = A + BTδ ,
we find that for I-a-N and I-b-S devices δ = 1.6 and 0.9,
respectively. In our case, µ ≈ T 1.6–0.9 for both the devices
indicating that charge carrier impurity scattering is the dom-
inating scattering mechanism over all the measured temperat-
ure range (T > 37 K). However, on lowering the temperature,
Figure 4. Charge carrier mobility as a function of temperature
estimated from fabricated I-a-N and I-b-S devices, respectively.
(a) natural m-MoS2 (I-a-N) flake and (b) synthetic m-MoS2 (I-b-S)
flake. Mobility values are fitted with the µ = A + BTδ function and
represented with solid lines. The best-fitting δ value is indicated as
the exponent of T.
the mobility keeps decreasing at a relatively slower pace, and
suddenly an apparent dip in the mobility appears around 37 K.
This anomalous behaviour can be understood on the basis of
freeze-out phenomenon of the charge carriers. It is to be noted
that the carrier freezeout phenomenon has been observed irre-
spective of the choice of the source of m-MoS2 flake (natural
or synthetic crystal). On lowering the temperature, the Fermi
level starts moving toward the conduction band edge. Possibly,
37 K represents the initiation of carrier freeze out in particular
impurity/defect state, beyond which mobility starts increasing
due to lowered concentration of charged impurities.
The mobility increases to a saturation level at temperat-
ures below 10 K owing to the scattering due to the resid-
ual impurities. Thus, 37 K can be considered as a crossover
point at which impurity concentration dependence of scat-
tering kicks in. The fact that we do not observe temperature
dependence due to phonon scattering mechanism seems reas-
onable since the carrier negotiates weak van der Waal potential
during transport. Earlier, many studies highlighted the role of
the orbital overlap of sulfur atoms in adjacent layers in gov-
erning the charge carrier transport in multilayer MoS2 . These
exfoliated flakes are known to have high defect density related
to sulfur (S) vacancies [44, 45]. The calculated mobilities are
in the range of 0.25–0.3 cm2 V−1 s−1 . Though the meas-
ured mobility values are lower in comparison to reported FET
(>100 cm2 V−1 s −1 ) and hall mobility values in few layer
samples (50–200 cm2 V−1 s −1 at room temperature) [29, 37].
But here it is to be noted that we have measured mobility of
charge carriers in micron size thick mechanically exfoliated
MoS2 flake where in perpendicular direction layers have larger
separation due to weak interactions. Therefore, the mobility is
likely to be lower than expected values purely due to impur-
ity and defect scattering. We attribute the observed behaviour,

5
J. Phys. D: Appl. Phys. 54 (2021) 295104
specifically the fact that the low carrier mobility is limited by
charge impurity scattering, to presence of defects, possibly the
S vacancies that inevitably occur in both the natural geological
and synthetic crystals.
4. Conclusions
In summary, we have measured the inter-layer mobility of
mechanically exfoliated multilayer MoS2 flakes for both nat-
urally occurring and synthetic crystals. Our results reveal that
inter-layer mobility in layered MoS2 is dominated by charged
impurity scattering decreasing with temperature till carrier
deionization of impurities sets in. Our ability to measure the
inter-layer mobility was made possible by the suitable choice
of device structure and utilization of the impedance spectro-
scopic technique based on Im (Z) eminently suitable for such
a measurement. A relatively lower mobility value in compar-
ison to reported intralayer mobility (50–200 cm2 V−1 s −1 )
is obtained, possibly due to the large inter-layer resistance
offered by the multiple layers. It could further be improved by
choosing the high purity MoS2 flake having low concentration
of impurity and defects. These results are not only signific-
ant to the design/functionalization of multilayer MoS2 based
applications, but also provide insight to direction depend-
ent transport properties of layered MoS2 that would lead to
enhanced performance of multilayer MoS2 based electronic
devices.
Data availability statement
The data that support the findings of this study are available
upon reasonable request from the authors.
Acknowledgments
The authors thank Manoranjan for his timely help on low tem-
perature measurements.
ORCID iDs
Shikha Srivastava  https://orcid.org/0000-0001-9961-5838
Yashowanta N Mohapatra  https://orcid.org/0000-0002-
7380-6027
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