Nano Research 2018, 11(2): 722–730

https://doi.org/10.1007/s12274-017-1681-5

High-performance multilayer WSe2 field-effect transistors

with carrier type control
Pushpa Raj Pudasaini1,2, Akinola Oyedele2,3, Cheng Zhang1,2, Michael G. Stanford1, Nicholas Cross1,
Anthony T. Wong1, Anna N. Hoffman1, Kai Xiao2, Gerd Duscher1,4, David G. Mandrus1,4, Thomas Z. Ward4,
and Philip D. Rack1,2 ()

1
Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, USA
2
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
3
Bredesen Center for Interdisciplinary Research and Graduate Education, University of Tennessee, Knoxville, TN 37996, USA
4
Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA

Received: 13 January 2017 ABSTRACT

Revised: 14 May 2017 In this study, high-performance multilayer WSe2 field-effect transistor (FET)
Accepted: 16 May 2017 devices with carrier type control are demonstrated via thickness modulation and
a remote oxygen plasma surface treatment. Carrier type control in multilayer
© Tsinghua University Press WSe2 FET devices with Cr/Au contacts is initially demonstrated by modulating
and Springer-Verlag GmbH
the WSe2 thickness. The carrier type evolves with increasing WSe2 channel
Germany 2015
thickness, being p-type, ambipolar, and n-type at thicknesses < 3, ~ 4, and > 5 nm,
respectively. The thickness-dependent carrier type is attributed to changes in
KEYWORDS
the bandgap of WSe2 as a function of the thickness and the carrier band offsets
transition metal relative to the metal contacts. Furthermore, we present a strong hole carrier
dichalcogenide, doping effect via remote oxygen plasma treatment. It non-degenerately converts
field-effect transistors, n-type characteristics into p-type and enhances field-effect hole mobility by three
carrier control, orders of magnitude. This work demonstrates progress towards the realization
plasma treatment,
of high-performance multilayer WSe2 FETs with carrier type control, potentially
carrier mobility
extendable to other transition metal dichalcogenides, for future electronic and
optoelectronic applications.

1 Introduction TMDs can exhibit semiconducting properties through

Recently, two-dimensional transition-metal dichalco-
genide (TMD) materials have received considerable
attention for their potential in nanoscale optoelectronic
device applications [1–4]. Unlike zero-bandgap graphene,
the proper selection of the transition metal and
chalcogen in the crystal, and their band gaps can be
tuned by manipulating the number of layers or thickness
[5–7]. It has been shown that the band structures of
TMD materials can exhibit unique indirect-to-direct

Address correspondence to prack@utk.edu

Nano Res. 2018, 11(2): 722–730
band gap transitions from bulk to single-layer structures
[6, 8]. For example, bulk WSe2 is an indirect-band-gap
(~ 1.2 eV) semiconductor, whereas monolayer WSe2
exhibits a direct band gap of ~ 1.65 eV [7, 9]. The
direct band gaps of single-layer TMDs offer exciting
opportunities for potential applications in both digital
electronics and optoelectronic devices [3, 10, 11]. WSe2
shows particular promise because n-type, p-type, and
ambipolar carrier transport can be achieved by thickness
modulation and electrode engineering [12, 13], which
is challenging for other TMD materials like MoS2
because of strong Fermi level pinning effects [14].
Carrier type control is essential to realize many
optoelectronic applications, and is vital to engineering
the n- and p-type transistor building blocks in com-
plementary metal-oxide semiconductor (CMOS) logic
gates [15, 16]. One of the fundamental challenges
realizing TMD-based CMOS-type devices is controlled
and reliable doping. TMD-based field-effect transistors
(FETs) typically show a dominant carrier transport
based on the native doping properties. For example,
MoS2 shows native n-type transport behavior [17, 18].
This intrinsic material property causes challenges in
modulating the carrier type in TMDs. Although many
works are ongoing in the field of doping TMDs, most
of them are limited to MoS2 [19–21], which forms a low
electron barrier contact with metals and is generally
used for n-channel transistors. Several different doping
mechanisms, such as cation substitution [17, 22],
interface dipole introduction [21, 23], and charge transfer
[24, 25], have been demonstrated to dope TMDs for
controlling carrier type and improving device per-
formance. Substitutional doping in particular is achieved
only during crystal growth, with limited control over
concentration. Carrier mobility in substitutionally doped
TMDs is significantly compromised by ionized
impurity scattering [17]. It has been shown that both
n- and p-type doping can be induced by exposing
TMDs to oxidizing or reducing species with suitable
redox potentials via surface charge-transfer methods
[26, 27]. For example, both p- and n-type doping
in MoS2 has been demonstrated via charge-transfer
methods using NH3 and NO2, respectively [28, 29].
Moreover, WSe2 has been p-doped via physisorbed
NO2. This doping scheme has achieved excellent p-type
FETs [30]; however, because of the non-covalent
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723
bonding nature of the adsorbed “dopant” molecules,
the strategy is limited by the dopant volatility over
time, which impedes control of the doping concen-
tration. Electrostatic doping has also been employed
to dope TMDs and many oxide materials using a
polymer electrolyte or ionic liquid gating, relying on
the applied voltage to modulate the carrier density
[31–34]. However, the challenge of stable and precise
carrier type control in TMDs remains.
In this work, we demonstrate high-performance
multilayer WSe2 FETs with carrier type control via
thickness modulation and remote oxygen plasma
surface treatment. The carrier type evolves from
p-type to ambipolar to n-type in WSe2 FETs devices
using Cr/Au contacts with increasing channel thickness.
Furthermore, we demonstrate the non-degenerate
p-type doping of few-layer WSe2 via remote oxygen
plasma surface treatment. The field-effect hole mobility
for the p-doped WSe2 FET is enhanced by more than
three orders of magnitude compared to that in the
pristine device without oxygen plasma treatment.
2 Experimental
Bulk single-crystal WSe2 was synthesized via a vapor
transport method from polycrystalline WSe2, as
described previously [4]. Few-layer WSe2 flakes were
mechanically exfoliated from the bulk crystals and
transferred on heavily doped p-type silicon substrates
with thermally grown 290-nm-thick SiO2 layers. The
transferred flakes were mapped in terms of location,
dimensions, and relative thickness using an optical
microscope. The thickness of the flakes was subsequently
measured via atomic force microscopy (AFM). The
substrates were then spin-coated with poly(methyl
methacrylate) (PMMA), and electron-beam lithography
(EBL) (FEI 600 Nova with Raith software) was employed
to define the source and drain pattern, followed by
metal evaporation and lift-off processes. An evaporation
rate of 1 Å/s was used for depositing metal contacts
of 5-nm Cr and 30-nm Au. The fabricated devices were
subjected to remote oxygen plasma surface treatments
in an atomic layer deposition tool (Oxford Instruments).
A radiofrequency power of 400 W and oxygen flow
rate of 60 sccm with 15-mTorr chamber pressure at
150 °C were employed for 60 s for the surface plasma
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724 Nano Res. 2018, 11(2): 722–730

treatment of WSe2 FET devices. Electrical charac-

terization was performed in a cryogenic probe system
with a semiconductor parametric analyzer (Agilent
Tech B1500 A). Scanning transmission electron
microscopy (STEM) imaging was performed with
a Nion UltraSTEM 200 operating at an accelerating
voltage of 200 kV. Flakes of WSe2 were exfoliated from
a bulk crystal onto SiNx grids. The sample was baked
at 160 °C in an inert atmosphere for 9 h directly prior
to imaging. The thin-flake WSe2 images consist of an
average of 20 frames each 512 × 512 pixels and a 4-μs
dwell time per pixel, using the high-angle annular
dark-field (HAADF) detector. Raman spectroscopy
was performed in a Renishaw inVia micro-Raman
system using a 532-nm excitation laser. A 50×
magnification objective lens was used for spectral
acquisition with a 3-s acquisition time.

3 Results and discussions

The few-layer WSe2 FET devices are fabricated with
different channel thicknesses (~ 1.5 to 23 nm) with
Cr/Au contacts, as shown in the schematic in Fig. 1(a).
An AFM image of one of the fabricated devices is
shown in Fig. 1(b). The height profile along the white
line in Fig. 1(b) is shown in Fig. 1(c), indicating a
~ 1.5-nm-thick (bilayer) WSe2 channel. The inset in the
upper left corner of the figure shows a corresponding
optical image of the device. Figure 1(d) shows the
typical transfer characteristics curves (IDS vs. VGS) of
the WSe2 FET devices at three different source-drain
voltages, i.e., VDS = 0.1, 0.6, and 1.1 V, for the three
representative WSe2 channel thicknesses of ~ 1.5, 3.5,
and 9.0 nm, respectively. The measured transfer
characteristics show clear thickness-dependent carrier
transport. Preferential p-type carrier transport is
observed for the device of ~ 1.5-nm (bilayer) WSe2
channel thickness (Fig. 1(d)), as well as a current on-off
ratio exceeding 106. As the thickness increases, the
transport behavior evolves from p-type to ambipolar.
Symmetric ambipolar carrier transport is observed
for the device having a five-layer, 3.5-nm-thick WSe2
channel (Fig. 1(d)). Figure 2 shows the measured IDS
vs. VDS curves demonstrating the ability to modulate
the WSe2 channel resistance for both negative and
positive gate bias voltages. A current on-off ratio
Figure 1 Fabrication of few-layer WSe2 FETs and corresponding
electric transport properties. (a) Schematic of the WSe2 FETs with
Cr/Au contacts. (b) AFM micrograph of one of the fabricated few-
layer WSe2 devices. (c) A height profile indicating the 1.5-nm-thick
WSe2 channel layer. Inset: optical micrograph of the same FET
device. (d) The transfer characteristic curves (IDS vs. VGS) for the
few-layer WSe2 FET devices with Cr/Au contacts, showing p-type
carrier transport (left panel, 1.5-nm-thick WSe2 FET), symmetric
ambipolar carrier transport (middle panel, 3.5-nm-thick WSe2 FET),
and n-type carrier transport (right panel, 9-nm-thick WSe2 FET),
respectively. (e) The thickness-dependent field-effect linear
mobilities for electrons and holes for few-layer WSe2 FETs with
Cr/Au contacts.
exceeding 106 for both n- and p-type conduction is
observed. With further increases in WSe2 thickness,
the transport behavior evolves from ambipolar to
n-type. Excellent n-type carrier transport is observed
for devices with 13-layer, ~ 9.0-nm-thick WSe2 flake
(Fig. 1(d)), resulting in a current on-off ratio of ~ 108.
The transport behaviors for all FET devices fabricated
with Cr/Au contacts and WSe2 channel thicknesses
ranging from 1.5 to 23 nm are shown in Fig. S1 in the
Electronic Supplementary Material (ESM). Figure 1(e)
shows the thickness-dependent field-effect mobility of
both electrons and holes for few-layer WSe2 devices
with Cr/Au contacts. The field-effect mobility is
extracted from the linear region of the device transfer

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Nano Res. 2018, 11(2): 722–730
characteristics as
 L  dI DS
    (1)
 W  C  VDC  dVGS
where L and W are the channel length and width and
C is the specific capacitance of the gate dielectrics.
The hole mobility is greater than the electron mobility
for thinner WSe2 channels (< 5 layers) and a maximum
hole mobility value of 4.86 cm2/(V·s) is observed for
the 3.5-nm-thick WSe2 device. This decreases to
0.07 cm2/(V·s) as the channel thickness is increased to
9.0 nm. Meanwhile, the electron mobility increases
with increasing thickness, with the maximum field-
effect mobility value of 71.0 cm2/(V·s) for the 9.0-nm-
thick WSe2 flake.
Figures 2(a)–2(d) show the thickness-dependent
output characteristics of few-layer WSe2 FETs for the
three different characteristic transport regimes. The
few-layer FET device fabricated using a 3.5-nm-thick
WSe2 channel shows ambipolar carrier transport, as
mentioned above. The source-drain current is increased
with the increase in gate voltage in both the negative
(Fig. 2(a)) and positive (Fig. 2(b)) gate bias regions.
Almost linear IDS–VDS behaviors are observed in both
the electron and hole transport regimes at small values
of applied drain voltage, suggesting nearly identical
barrier heights for both electrons and holes between
the Cr contacts and the 3.5-nm WSe2 channel. This is
further confirmed by the nearly equal values of onset
voltage for both p-type (~ −20 V) and n-type (~ 16 V)
transport regimes at a small applied drain voltage
(0.6 V) (transfer curve Fig. 1(d)), suggesting that
the Cr Fermi level lies close to the middle of the
3.5-nm-thick WSe2 bandgap. The onset voltage is
defined as the gate voltage leading to a 1-nA channel
current in the device. The thickness-dependent bandgap
values of WSe2 have been extensively reported in the
literature, with ~ 1.67 eV for a single layer and ~ 1.2 eV
for the bulk WSe2 crystal [7]. The layer-dependent
energy levels of the valance band maxima (VBM) and
conduction band minima (CBM) are also reported
in the literature. The previous experimental result
shows the VBM/CBM values of −4.03 eV/−5.18 eV
in eight-layer WSe2 [35]. The relationship between
the number of layers and the VBM/CBM values was
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725
theoretically calculated by Zhou et al. through a
density functional theory method [36]. By applying
this slope of layer number vs. the VBM/CBM values
and considering other reported results [37], we
extrapolated and estimated the VBM/CBM values for
our five-layer device as −3.98 eV/−5.22 eV. Based on
the VBM/CBM energies for five-layer WSe2 and the
observed symmetric ambipolar transport (Fig. 1(d)) of
the corresponding FET device, we assume the work
function of Cr lies in the middle of the band gap of
the five-layer WSe2, i.e., ~ 4.6 eV, when in contact with
the WSe2 crystal. The resulting band offset between
the five-layer WSe2 and Cr metal electrode is shown
in the inset of Figs. 2(a) and 2(b). An experimental
report showed that the band gap of bilayer WSe2 was
1.44 eV [38]. Considering the theoretical calculation
showing that the absolute VBM value for bilayer
WSe2 is 0.042 eV lower than that of the five-layer
WSe2 [36], we can estimate the VBM/CBM values as
−3.83 eV/−5.26 eV for our bilayer device, as shown in
Fig. 2(c), which is consistent with the p-type conduction
observed. This favorable band alignment for hole
transport is consistent with the observed preferential
p-type carrier transport in the bilayer ~ 1.5-nm-thick
WSe2 FET device (Figs. 1(d) and 2(c)). The energy
band offset diagram for bulk (~ 9 nm) WSe2 device
is shown in the inset of Fig. 2(d). The linear IDS–VDS
behavior seen in Fig. 2(d) shows the small resistance
of ~ 36 kΩ in the n-type transport regime, and a large
negative shift (~ 15 V) in the onset voltage compared
to that of the ambipolar transport (Fig. 1(d)) device.
This suggests possible native n-type doping in bulk
WSe2. Furthermore, the Fermi level in the bulk WSe2
sample may have shifted while in contact with the
metal Cr electrodes. A similar observation was reported
for bulk WSe2 in contact with Ag via atomistic
simulations [13]. Carrier type controlled by thickness
modulation in few-layer WSe2 devices was also recently
demonstrated using Ni contacts [36]. The ambipolar-
to preferential-n-type carrier transport transition was
reported for relatively thick WSe2 channels (~ 15 nm),
consistent with the high work function of Ni contacts.
Relatively weakly (less than three orders) preferential
n-type transport with a small current on–off ratio (~ 104)
was observed in devices with Ni contacts compared
to those with the Cr contacts reported herein, which
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726 Nano Res. 2018, 11(2): 722–730

Figure 2 Thickness-dependent electrical transport properties for few-layer WSe2 FET devices. (a) and (b) The output characteristic
curves (IDS vs. VDS) for WSe2 FET with 3.5-nm channel thickness, showing ambipolar carrier transport. The source-drain channel
currents increase with increasing gate voltage both in (a) negative and (b) positive gate bias. The IDS vs. VDS curves for (c) p-type 1.5-nm
and (c) n-type 9.0-nm channel-thickness WSe2 FET devices.

showed a promising current on–off ratio exceeding 108.
Other groups have also reported preferential p-type
and n-type carrier transport in few-layer WSe2 FET
devices employing different contacts of high-work-
function metals, such as Pt [39] and Pd [40], and
low-work-function metals, such as In and Ag [13],
respectively. These reports are also in line with our
transfer measurement for the devices using Pd contacts,
because Pd has a higher work function than Cr, as
shown in Fig. S2 in the ESM. Interestingly, unlike Cr
contacts for few-layer WSe2 FET devices, we do not
observe thickness-dependent carrier type transport
for WSe2 devices with Ti/Au contacts. We observe
ambipolar behavior irrespective of the WSe2 channel
thickness (see Fig. S3 in the ESM). This might be due
to the oxidation in the contact interfaces, as has been
reported previously [41, 42]. The non-metallic contact
between Ti and TMD leads to a more complex situation
in which the Schottky barrier height is not determined
by the metal’s work function. Further investigations
are needed.
In addition to the thickness-dependent study in WSe2
devices presented above, we further employ a remote
oxygen plasma surface treatment method to realize
non-degenerate p-type doping. Figure 3 shows the
transfer curves of a few-layer WSe2 device before
(Fig. 3(a)) and after (Fig. 3(b)) oxygen plasma treatment.
The initial preferential n-type characteristics (Cr/Au
electrodes, ~ 7 nm WSe2 channel) are changed to p-type
after the oxygen plasma treatment. The on-state current
for the hole transport is increased by almost four
orders of magnitude, yielding a promising current
on–off ratio exceeding 109. The field-effect hole mobility
increases from 0.13 to 117.89 cm2/(V·s), while the electron
mobility decreases from 11.35 to 0.0048 cm2/(V·s). The
hole doping effect on few-layer WSe2 by oxygen plasma
surface treatment is clearly observed in all devices,
regardless of channel thickness. For the device with

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Nano Res. 2018, 11(2): 722–730 727

Figure 3 Oxygen plasma treatment effect on electrical characteristics of few-layer WSe2 FET devices. The transfer characteristics for
few-layer WSe2 FET devices, (a) before (pristine device) and (b) after oxygen plasma surface treatment. The initial preferential n-type
carrier transport in the few-layer WSe2 device is changed to strong p-type carrier transport, with an increase by more than three orders of
magnitude in currents in the hole transport regime after oxygen surface plasma treatment. (c) Transfer curves of the same device
(plasma-treated), measured after 90 days of storage in ambient conditions, indicating that the described plasma-induced doping is very
stable. (d) Comparison of transfer curves for the device before, right after, and aged after the surface plasma treatment, measured at
different times at VDS = |1.1| V.

a relatively thin WSe2 channel (below 7.0 nm), the
initial ambipolar or n-type characteristic of the device
is converted to a strong p-type characteristic. For
the device with a thicker WSe2 channel, the initial
preferential n-type characteristic is changed to ambipolar
transport characteristics with an increase of up to
four orders of magnitude in the current in the hole
transport regime (see Fig. S4 in the ESM). The plasma-
induced p-doping observed herein is attributed to
charge-transfer doping reported elsewhere [24]. For
the thicker WSe2 channel devices, the described hole
doping via remote oxygen plasma surface treatment
occurs only in the top few-layers, while the bottom
layers still support electron conduction. Therefore, the
initial n-type carrier transport is changed to ambipolar
carrier transport after plasma exposure. Previously
reported charge-transfer doping in TMD was very
unstable, decaying almost completely within a couple
of hours [26, 35]. However, the plasma-induced
doping describe herein is relatively stable. Figure 3(c)
shows the transfer characteristic curves of the same
plasma-treated device measured after 90 days of
storage in ambient conditions, which indicate that the
charge-transfer doping process is stable. A small (< 5%)
change in the on-state current in the hole transport
regime is observed after 90 days, with an almost
identical current on–off ratio exceeding 109 (Fig. 3(d)).
The plasma-assisted processing of two-dimensional
TMD materials in general typically produces undesirable
side effects such as layer etching, surface oxidation,
and the degradation of material quality. Yamamoto el
al. [43] reported that exposing thin WSe2 films to
ozone at 100 °C caused self-limiting oxidation of the
WSe2 surfaces, which acted as a p-type layer. To check
the possible surface oxidation and substantial oxygen
doping by the remote oxygen plasma surface treatment,
we collected high-resolution STEM images of a
suspended WSe2 layer exposed to an identical remote
oxygen plasma treatment. Figures 4(a) and 4(b) depict
the HAADF STEM images of the layer before and
after exposure to the oxygen plasma treatment. The
insets in the lower right corner show the corresponding
selected-area diffraction patterns. Ostensibly, no disorder
or defects are observed from the plasma exposure.
Electron energy-loss spectroscopy (EELS) results,
acquired moving from the edge of the sample toward
the center, are shown in Fig. 4(c). A small oxygen signal
is observed (the oxygen K-shell ionization edge has
an onset energy of 532 eV) at the very edge of the
sample (Fig. 4(d)), but quickly vanishes as the beam
moves toward the center. This demonstrates that slight
oxygen doping is isolated in the defective edge regions
of the WSe2 flake, and that no further doping occurs
away from the edge during the plasma surface treatment
process. This is also confirmed by the virtually identical
Raman spectra acquired for the few-layered WSe2
sample both before and after remote oxygen plasma
surface treatment (see Fig. S5 in the ESM).

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728
Figure 4 HAADF STEM images for suspended few-layer WSe2
samples. STEM micrographs of the (a) pristine and (b) oxygen
plasma surface-treated few-layer WSe2 samples. Insets in the lower
right corners: corresponding selected-area diffraction patterns. No
noticeable plasma-induced structural disorder or defects in the
materials are observed. (d) EELS image scan acquired in different
areas from the edge of the sample shown in (c). A small oxygen
signal (green curve) at the very edge can be seen, but quickly
vanishes as the center is approached, suggesting no oxygen doping
of WSe2 occurs during plasma exposure.
4 Conclusion
In summary, carrier type control in few-layer WSe2
FET devices with Cr/Au contacts is demonstrated by
WSe2 channel thickness modulation and remote oxygen
plasma treatment. It is observed that the transport
behavior is directly related to the WSe2 channel
thickness, specifically evolving from p-type (< 3 nm)
to ambipolar (~ 4 nm) to n-type (> 5 nm). Strong and
non-degenerate hole carrier doping is also realized by
remote oxygen plasma surface treatment. The field-
effect hole mobility of the oxygen plasma-treated WSe2
FET devices is increased by three orders of magnitude
relative to that of the pristine device. The described
method for the carrier type control in few-layer WSe2
via thickness modulation as well as oxygen plasma
surface treatment could be practically applied in FETs
in integrated circuits.
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Nano Res. 2018, 11(2): 722–730
Acknowledgements
P. D. R. and M. G. S. acknowledge support by U.S.
Department of Energy (DOE) under Grant No. DOE
DE-SC0002136. P. R. P. and D. G. M. acknowledge
funding by the Gordon and Betty Moore Foundation’s
EPiQS Initiative through Grant GBMF4416. T. Z. W.
acknowledges support U.S. Department of Energy
(DOE), Office of Basic Energy Sciences (BES),
Materials Sciences and Engineering Division. A. T. W.
acknowledges support by Laboratory Directed Research
and Development Program of Oak Ridge National
Laboratory, managed by UT-Battelle, LLC, for the U.S.
Department of Energy. N. C. acknowledges support
by National Science Foundation (NSF) (No. DMR-
1410940). The authors acknowledge that the device
synthesis and Raman mapping were conducted at the
Center for Nanophase Materials Sciences, which is a
DOE Office of Science User Facility.
Electronic Supplementary Material: Supplementary
material (additional electrical and Raman spectra
measurements data) is available in the online version
of this article at https://doi.org/10.1007/s12274-017-
1681-5.
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