pubs.acs.

org/NanoLett Letter

Ultrasensitive Phototransistor Based on WSe2−MoS2 van der Waals

Heterojunction
Gwang Hyuk Shin,† Cheolmin Park,† Khang June Lee, Hyeok Jun Jin, and Sung-Yool Choi*
Cite This: Nano Lett. 2020, 20, 5741−5748 Read Online

ACCESS Metrics & More Article Recommendations *

sı Supporting Information
See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.
Downloaded via XIDIAN UNIVERSITY on October 18, 2022 at 13:13:07 (UTC).

ABSTRACT: Band engineering using the van der Waals heterostructure of two-dimensional materials allows for the realization of
high-performance optoelectronic devices by providing an ultrathin and uniform PN junction with sharp band edges. In this study, a
highly sensitive photodetector based on the van der Waals heterostructure of WSe2 and MoS2 was developed. The MoS2 was utilized
as the channel for a phototransistor, whereas the WSe2−MoS2 PN junction in the out-of-plane orientation was utilized as a charge
transfer layer. The vertical built-in electric field in the PN junction separated the photogenerated carriers, thus leading to a high
photoconductive gain of 106. The proposed phototransistor exhibited an excellent performance, namely, a high photoresponsivity of
2700 A/W, specific detectivity of 5 × 1011 Jones, and response time of 17 ms. The proposed scheme in conjunction with the large-
area synthesis technology of two-dimensional materials contributes significantly to practical photodetector applications.
KEYWORDS: photodetector, MoS2, WSe2, van der Waals heterostructure, phototransistor

1. INTRODUCTION monolayer MoS2 phototransistors exhibit a high responsivity of

Photodetectors are critical elements in state-of-the-art
technologies, which include autonomous vehicles, environ-
mental monitoring systems, security systems, mobile phone
cameras, and telecommunications systems. In particular,
complementary metal oxide semiconductor (CMOS) image
sensors are widely used in digital cameras due to their low-
power consumption and low cost. Each pixel of an CMOS
image sensor comprises a PN photodiode, amplifier circuit,
and switching transistor. The PN diode collects the electron
generated by the light, and the electrons change the voltage of
the capacitor, whereas the peripheral transistors amplify the
voltage. These external circuits can be simplified using
phototransistors, which facilitate the conversion from the
photon to electron−hole pair and the amplification of the
photoconductive gain with an external quantum efficiency
(EQE) that exceeds 100%.1−5
Two-dimensional (2D) semiconductors have attracted
significant research attention with respect to photodetectors,
due to their superior optical and electrical properties.6−11 In
particular, MoS2 phototransistors have been investigated with
respect to various structures and mechanisms.12−24 Although
880 A/W, the response time is within a range of several
seconds due to trap states around the channel.20 Moreover,
MoS2 phototransistors based on photosensitizing schemes have
been investigated, which operate as in-plane phototransistors
with out-of-plane vertical PN junctions, and demonstrate
excellent performances with respect to a responsivity of 7 ×
104 A/W, specific detectivity of 1014 Jones, and a response time
of several milliseconds.17 The chemical doping of AuCl3 on the
surface of a MoS2 transistor was carried out for the formation
of the PN homojunction. The variations in the spatial random
dopant may result in device-to-device performance variations
with respect to large-area array applications.
Received: April 3, 2020
Revised: June 25, 2020
Published: June 26, 2020

© 2020 American Chemical Society https://dx.doi.org/10.1021/acs.nanolett.0c01460

5741 Nano Lett. 2020, 20, 5741−5748
Nano Letters pubs.acs.org/NanoLett
Figure 1. Phototransistor based on WSe2−MoS2 van der Waals heterojunction. (a) Optical microscopy image of phototransistor with Ni as source
and drain electrode. (b) Atomic force microscopy image of device based on WSe2 and MoS2 with 9 nm. (c) Raman spectra of the heterojunctions
of WSe2−MoS2, WSe2, and MoS2. (d) Schematic diagram of the device under laser irradiation at the heterojunction.
The stacking of 2D semiconductors allows for the formation
of van der Waals heterostructures, which have spatially uniform
PN heterojunctions with low trap states. Hence, various
heterostructures of 2D semiconductors were investigated for
carrier transport and photonics.25−45 For example, WSe2−
MoS2 van der Waals PN heterostructures have been
investigated with respect to electron and hole carrier
transport.36,40,44 Although WSe2−MoS2 heterostructures dem-
onstrate excellent physical properties, limited research has been
conducted on optoelectronic devices for practical applications.
In this study, a high-performance phototransistor based on
WSe2−MoS2 van der Waals heterostructures with a photo-
sensitizing scheme was developed. The phototransistor exhibits
a high responsivity (R) of 2700 A/W, specific detectivity (D*)
of 5 × 1011 Jones, and response time of 17 ms. The WSe2−
MoS2 heterostructure offers several advantages for the
photodetector. First, a high photocurrent with dozens of
microamperes (μA) could reduce the complexity of the sensing
circuit as the addition of the amplification circuit becomes
unnecessary. Second, it shows a broader spectral response
compared to a single MoS2 channel due to the absorption
resonance of WSe2. Third, an atomically uniform and thin film
without-doping process not only simplifies the fabrication
process but also enables the image sensor array to be of high
resolution. In the proposed device, MoS2 acts as the main
conduction channel; whereas, the heterojunction region of
WSe2−MoS2 acts as a photosensitizer, given that the WSe2−
MoS2 heterojunction forms type-II staggered structures in the
out-of-plane direction. The built-in potential of the PN
junction creates an electric field, thus resulting in the
separation of the photoinduced electron−hole pairs. Con-
sequently, the PN junction enhances the lifetime of the charge
carrier and photogain. In addition, the van der Waals structure
provides spatial uniformity and a clean interface with low trap
5742
Letter
states. Therefore, the WSe2−MoS2 van der Waals hetero-
structure can serve as suitable channel materials for high-
performance photodetectors.
2. RESULTS AND DISCUSSION
The MoS2 flakes with several layers were exfoliated onto the 90
nm-SiO2/Si substrate by a micromechanical cleavage technique
using adhesive tape. The WSe2 flakes with several layers were
then exfoliated onto another 90 nm-SiO2/Si substrate. For the
development of the van der Waals heterojunction of WSe2 and
MoS2, MoS2 flakes with several layers were transferred onto the
WSe2 flakes with several layers using the pick-up transfer
method. Thereafter, the 50 nm-Ni electrodes were patterned
using e-beam lithography and deposited using a thermal
evaporator (see the Supporting Information, Figure S1). The
optical microscope and atomic force microscope images of the
phototransistor based on the van der Waals heterojunction of
WSe2 and MoS2 are shown in Figures 1a and b, respectively.
The thicknesses of the WSe2 and MoS2 layers were measured
as 9 nm, respectively. The total thickness of the device was 18
nm, thus indicating that the WSe2−MoS2 PN junction in the
out-of-plane direction of the channel contained approximately
24 layers. Moreover, several devices were fabricated with PN
junctions of various thicknesses, to verify the optimized
performance. The thickness of 9 nm-WSe2 and MoS2 layers
resulted in the highest performance among the devices. We
designed the thickness of MoS2 and WSe2 in accordance with
the depletion layer model for a conventional PN junction
heterostructure (see the Supporting Information, Figure S2).
By the stacking of the WSe2 onto MoS2, the PN heterojunction
was formed without doping techniques, given that WSe2 and
MoS2 are intrinsically p-type and n-type semiconductors.
Hence, an atomically uniform PN junction can be developed.
In addition, the van der Waals heterojunction provides a high-
https://dx.doi.org/10.1021/acs.nanolett.0c01460
Nano Lett. 2020, 20, 5741−5748
Nano Letters pubs.acs.org/NanoLett Letter

Figure 2. Electrical I−V characteristics of the phototransistor based on the WSe2−MoS2 van der Waals heterojunction under the nonillumination
condition. (a) IDS−VGS transfer characteristics at drain voltages of 0.01−5 V. (b) IDS−VDS output characteristics at gate voltages of −10 to 10 V.

Figure 3. Photoresponse of a phototransistor based on the WSe2−MoS2 van der Waals heterojunction. (a) Spatial map of the photocurrent
measured by conducting scan over the surface of the device using a focused laser beam (scale bar: 10 μm) at VDS = 5 V, VGS = −5 V, and Pinc = 2
μW. (b) Energy band diagram of the WSe2−MoS2 van der Waals PN heterojunction with photogenerated carriers under focused laser beam
irradiation. (c) Photoresponse of the IDS−VGS transfer characteristics under nonillumination and illumination conditions, obtained for a back-gate
voltage in the range of −20 to 20 V and drain voltage of 5 V. The illumination wavelength was 532 nm, and the power increased from 0.005−1 μW.
(d) Photocurrent as a function of wavelength from 450−800 nm, thus exhibiting a broad band spectral response for VDS = 5 V, VGS = −5 V, and Pinc
= 50 μW.

quality interface, in addition to low trap states and defects
without lattice mismatch. Figure 1c presents the Raman
spectra of a sample at different positions, namely, the
heterojunctions of WSe2 and MoS2, WSe2, and MoS2. The
spectrum of WSe2 exhibited one strong peak at 248 cm−1 and
two weak peaks at 371 and 392 cm−1, respectively. Moreover,
in the MoS2 region, there were two strong peaks at 380 and
404 cm−1. However, the intensities of the MoS2 peaks were
reduced at the heterojunction of WSe2 and MoS2. This can be
5743
attributed to the strong interfacial coupling between WSe2 and
MoS2, which generated the charge transfer, thus resulting in
the reduction of the Raman intensity.40 A similar quenching
effect was confirmed in the photoluminescence spectra of the
same sample (see the Supporting Information, Figure S3).
Figure 1d presents the schematic of the device under the
illumination of a focused laser beam. The photoresponse of the
device was measured due to laser irradiation on the
heterojunction. The spot size of the laser beam was about 1
https://dx.doi.org/10.1021/acs.nanolett.0c01460
Nano Lett. 2020, 20, 5741−5748
Nano Letters pubs.acs.org/NanoLett Letter

Figure 4. Dependence of photoresponse on gate voltage and illumination intensity. (a) Photoresponsivity of the transistor based on the WSe2−
MoS2 van der Waals heterojunction, thus indicating a high responsivity of 2700 A/W at an illumination power of 5 nW and gate voltage of 20 V, for
VDS = 5 V, VGS = −10 to 20 V, and wavelength of 532 nm. (b) Specific detectivity of the device as a function of the gate voltage from −2.5 to 20 V
for VDS = 5 V and Pinc = 5 nW. (c) Photocurrent and (d) photoresponsivity of the device as a function of the incident laser power from 0.005−1
μW, for VGS = 20 V, VDS = 5 V, and Pinc = 5 nW.

μm. In the device structure, the MoS2 is the main conduction
channel, whereas the heterojunction of WSe2 and MoS2 acts as
a photosensitizer, which enhances the separation of the
photogenerated carriers due to the built-in voltage of the PN
junction in the vertical direction. Moreover, the WSe2 is
isolated from the source and drain contact.
To investigate the I−V characteristics of the transistor, the
transfer IDS−VGS and output IDS−VDS characteristics under
nonillumination were determined. Figure 2a presents the back-
gate modulated transfer characteristics of the device, which
indicates the transport properties of the carriers. At the
negative gate voltages from −20 V to −10 V, the drain current
was suppressed at a low drain voltage of 0.01 V; however, it
increased in accordance with an increase in the drain voltage
from 0.05−5 V. The hole carriers from WSe2 are injected into
the MoS2 channel when the gradient of the MoS2 energy band
is changed by the drain voltage. At a gate of −10 to 0 V, the
drain current exhibited negative differential resistance (NDR)
characteristics. This can be attributed to the decrease in the
majority carriers of the main conduction channel of the MoS2
due to recombination between the electrons in the MoS2 and
holes in the WSe2. Similar results for the NDR of the transistor
based on the heterostructure were reported.36,37,40 At a gate
voltage of 0−20 V, the drain current exhibited the typical
characteristics of an MoS2-based transistor. In this region,
WSe2 are depleted, whereas MoS2 electrons are accumulated.
In general, with an increase in the drain voltage, the drain
current increased due to its proportional relationship with the
electric field between the source and drain. This charge
transport mechanism can be explained by the energy band
5744
diagram (see the Supporting Information, Figure S4). The field
effect mobility of the device was found to be 8.42 cm2/V·s
based on the maximum transconductance (gm) method. The
gate capacitance Cg = 3.71 × 10−8 F/cm2 for the 90 nm thick
SiO2 layer and 9 nm WSe2 layer was used in the mobility
calculation. Figure 2b presents the output I−V characteristics,
in which the drain current gradually increased at drain voltages
between −1 and 1 V in accordance with an increase in the gate
voltage from −10 to 10 V. The inset figure presents the Ohmic
characteristics of the device. Moreover, the results indicate that
the MoS2 conduction channel is effectively modulated by the
back-gate, whereas the screening effect of WSe2 is negligible.
The optoelectronic characteristics of the device were then
evaluated under the irradiation of a focused laser beam (λ =
532 nm). The diameter of the laser beam spot is recorded as
872 nm by the formula of d = k(λ/NA), where k = 0.82 for the
Gaussian beam shape and the NA is 0.5, which is small enough
to illuminate on the WSe2−MoS2 heterostructure. Figure 3a
presents the spatially resolved photocurrent map obtained
from a scan conducted over the surface of the device using a
positioning stage. The photocurrent was measured at the
heterojunction of WSe2 and MoS2, thus indicating that the
photogenerated carriers in the PN junction were effectively
separated by the built-in electric field. The photovoltaic effect
was observed at a gate and drain voltage of 0 V, thus
confirming that the PN junction was well-formed in the device
(see the Supporting Information, Figure S5). Information on
the equipment used for the photocurrent mapping is shown in
Figure S5. Figure 3b presents the energy band diagram of the
PN junction under laser beam irradiation in the out-of-plane
https://dx.doi.org/10.1021/acs.nanolett.0c01460
Nano Lett. 2020, 20, 5741−5748
Nano Letters pubs.acs.org/NanoLett Letter

Figure 5. Photoresponse dynamics. (a) Time-resolved photoresponse of the device, thus indicating excellent ON/OFF switching characteristics,
which were achieved using an optical chopper with a frequency of 5 Hz, for VGS = −5 V, VDS = 5 V, and Pinc = 400 nW. (b) Response time as a
function of the gate voltage, inclusive of the rise and decay time. (c, d) Energy band diagram of MoS2 under illumination conditions upon the
application of gate voltages below and above the threshold voltage. The gate-voltage-dependent response time can be explained by the energy band
diagram with trap states, where CB is the conduction band, VB is the valence band, and EF is the Fermi-level.

direction. When the focused laser beam irradiation was
incident on the heterojunction of WSe2 and MoS2, the
electrons in WSe2 were transferred to MoS2, whereas the holes
in MoS2 were transferred to WSe2. This resulted in the
photogating effect, wherein the charges modulated the
conductance of the MoS2 channel. Figure 3c presents the
photoresponse of the IDS−VGS transfer curve at a drain voltage
of 5 V under the focused laser beam irradiation within a power
range of 5 nW−1 μW, (λ = 532 nm). At gate voltages greater
than −10 V, the photocurrent (IPH = Iilluminated − Idark)
gradually increased in accordance with an increase in the
incident laser power. As the illumination laser intensity
increases, the number of photoexcited carriers increases, and
they are separated by the WSe2 and MoS2 PN heterojunction.
Hence, the magnitude of the photocurrent is enhanced with
increasing incident power. With an increase in the electric field
strength between the source and drain, the drift velocity of the
photogenerated electrons in the MoS2 channel increased, thus
resulting in a decrease in the carrier transit time Ttransit. In
l2
particular, Ttransit = , where l, μ, and VDS are the length
μVDS
between the source and drain, carrier mobility, and drain
voltage, respectively. The carrier transit time of the device was
calculated as 25 ns. A shift in the threshold voltage indicates a
photogating effect where charges separated from the PN
junction modulate the conductance of the MoS2 channel.
Figure 3d presents the spectral photocurrent response of the
device at wavelengths of 450−800 nm, bias of VGS = −5 V, VDS
= 5 V, and Pinc = 50 μW. Two peaks were observed at 680 and
760 nm, which correspond to photon energies of 1.8 and 1.6
eV, in addition to the bandgaps of MoS2 and WSe2,
5745
respectively. For energy band structures of multilayer MoS2
and WSe2, the conduction band minimum and valence band
maximum for different values of momentum are located along
the Γ−K direction, which means that the indirect-gap
transition is dominant.46 However, the direct-gap transition
can also be realized at the K or H point of the Brillouin zone
between the conduction and valence bands with relatively
lower quantum efficiency compared to the monolayer MoS2
and WSe2, which are direct-gap materials.46 In addition, we
observed the photoluminescence spectra as shown in Figure
S3, which provides evidence of direct transition in WSe2 and
MoS2. Therefore, it is considered that the absorption
resonances occur at laser wavelengths of 680 and 760 nm.
Photoresponsivity is a significant figure of merit for a
photodetector. Figure 4a presents the photoresponsivity at
different gate voltages and incident laser powers. The
wavelength of the laser was 532 nm, and a drain voltage of 5
V was applied. The photoresponsivity was determined as the
ratio of the photocurrent (IPH) to the incident laser power
(Pinc), i.e., or (IPH /Pinc). At gate voltages of −10 to 5 V, the
photoresponsivity increased in accordance with an increase in
the gate voltage. However, saturation was reached at a gate
voltage of 5 V. When the electrons were accumulated in the
MoS2 channel by the modulation of the back-gate voltage,
traps states were occupied by the electrons, thus enhancing the
conversion efficiency of the light to electrons. The device
demonstrated a high photoresponsivity of 2700 A/W at a laser
power of 5 nW. This value is higher than or comparable with
those reported in previous studies on phototransistors based
on 2D materials. The PN heterojunction of WSe2 and MoS2
https://dx.doi.org/10.1021/acs.nanolett.0c01460
Nano Lett. 2020, 20, 5741−5748
Nano Letters
was found to delay the recombination of photogenerated
carriers due to the built-in electric field. Hence, the lifetime of
the photogenerated carriers and the photoconductive gain
increased, which resulted in a high photoresponsivity.
Detectivity is a significant figure of merit for a photodetector.
The specific detectivity was plotted at the different gate
voltages, as shown in Figure 4b. The specific detectivity is
defined as D* = R(A/2qIdark)1/2, where R, A, q, and Idark are the
photoresponsivity, effective device area, element charge, and
dark current, respectively. Moreover, only the shot noise was
considered as the main noise source. The device demonstrated
a maximum detectivity of D* = 5 × 1011 Jones, which is also
higher than or comparable with those reported in other
studies.1,12−14,17,20,22,27 Figure 4c presents the photocurrent as
a function of the incident laser power. With an increase in the
intensity of the laser power, the photocurrent exhibited a
sublinear dependence. This can be attributed to the traps states
near the MoS2 channel.20 Figure 4d presents the photo-
responsivity with respect to the incident laser power. With a
decrease in the intensity of the incident laser power, the
photoresponsivity increased. Although the measurements were
conducted at a minimum intensity of 5 nW due to the
limitations of the measurement instrument, the photo-
responsivity of the proposed device is expected to increase at
lower intensities of the incident laser power. The photocurrent
and photoresponsivity as a function of the incident power were
measured at a bias of VGS = 20 V, VDS = 5 V, and Pinc = 5 nW.
To better understand the carrier dynamics under the laser
beam irradiation, time-resolved measurements were con-
ducted, as shown in Figure 5a. The ON/OFF switching of
the laser beam was realized by the optical chopper at a
frequency of 5 Hz. The device exhibited excellent switching
characteristics with an ON/OFF ratio of over 102 and a
response time of 30 ms at the bias of VGS = −5 V, VDS = 5 V,
and Pinc = 400 nW. The time-resolved photoresponse was
measured at various gate voltages (see the Supporting
Information, Figure S6). Figure 5b presents the response
time as a function of the gate voltage. With an increase in the
gate voltage from −10 to 10 V, the rise and the decay time of
the device decreased. At a gate voltage of 10 V, the rise time
was measured as 17 ms, which is lower than those reported for
other phototransistors based on 2D materials.1,12−14,17,20,22,27
T
Based on the results, a photoconductive gain, G = T life , was
transit
calculated, where Tlife and Ttransit are the carrier lifetime and the
transition time, respectively. The carrier lifetime and transition
time were 30 ms and 25 ns, which resulted in a photo-
conductive gain of 106. Physical parameters for the calculation
of the photoconductive gain are summarized in the Supporting
Information, Table S7. This high gain allowed for the
realization of the high photoresponsivity of 2700 A/W.
Moreover, the gate-dependent response time can be described
by the energy band model, as shown in Figures 5c and d. When
the gate voltage was lower than the threshold voltage (VTH),
there were unoccupied trap states, which resulted in the
retardation of the response time. However, when the gate
voltage was higher than the VTH, the trap states were occupied,
which resulted in a decrease in the response time. In a previous
study conducted on the carrier dynamics within the photo-
detector, the trapping/detrapping rate was found to be related
to the number of filled traps based on the rate equation.47
pubs.acs.org/NanoLett Letter
3. CONCLUSIONS
In this study, an ultrasensitive photodetector based on the van
der Waals heterostructures of WSe2 and MoS2 was developed,
which utilizes the band engineering in the vertical direction
without a doping technique. This out-of-plane PN junction
enhances the photoresponsivity by separating the photo-
generated carriers, thus resulting in an increase in the carrier
lifetime and photoconductive gain. The photodetector based
on the van der Waals heterostructures of WSe2 and MoS2
demonstrated an excellent performance, namely, a photo-
responsivity of 2700 A/W, specific detectivity of 5 × 1011, and
response time of 17 ms; which are higher than or comparable
to those reported in previous studies (see the Supporting
Information, S8).1,12−14,17,20,22,27 In addition, the photocurrent
with respect to the wavelength of the laser exhibited a broad
spectral range sensitivity for wavelengths of 450−800 nm. The
findings of this study in conjunction with a large-area synthesis
technique such as chemical vapor deposition (CVD) and liquid
exfoliation method can serve as a basis for the development of
practical photodetector applications, thus expanding the
research scope for optoelectronic devices based on van der
Waals heterostructures.
4. EXPERIMENTAL SECTION
4.1. Device Fabrication. The MoS2 and WSe2 crystals
were sourced from the 2D Semiconductors Corporation. The
90 nm SiO2 wafers were sourced from Namkang Hi-Tech. The
several layers of MoS2 and WSe2 flakes were obtained by the
mechanical cleavage technique using adhesive tape. After the
fabrication of the heterojunction, electron beam (e-beam)
lithography was conducted on the source and drain pattern,
followed by 50 nm Ni evaporation using a thermal evaporator.
The lift-off technique was conducted in acetone for 10 min at
60 °C. The devices were then annealed at 150 °C for 2 h in a
vacuum, for the improvement of the contact quality (see the
Supporting Information, Figure S1).
4.2. Pick-up Transfer Method. A polypropylene carbo-
nate (PPC) solution of 6 w% was prepared by dissolving the
PPC in chloroform. The solution was spin-coated on a target
sample at 3000 rpm for 30 s. Thereafter, the sample was
annealed on a hot plate for 30 s at 90 °C in air. Thereafter, a
polydimethylsiloxane (PDMS) stamp was attached on the
sample with the PPC. Using pick-up transfer equipment, which
included an optical microscope, heater, and micropositioner,
the transfer was conducted onto another target sample. The
sample was subjected to a temperature of 90 °C for the
detachment of the PDMS. The PPC on the sample was then
removed by immersion in acetone for 10 min.
4.3. Device Characterization. All the measurements were
conducted under ambient conditions using a semiconductor
parameter analyzer (4200 SCS, Keithley Instruments). The
semiconductor diode laser beam with a wavelength of 532 nm
was focused onto the channel area in the device using an
objective lens with a long operating distance and magnification
of 50× (NA 0.5). The spectral responsivity was measured
using a supercontinuum laser (SuperK Extreme, NKT
Photonics) and monochromator. To maintain a constant
intensity within the spectral range for an accurate measure-
ment, a power table was developed for the control of the
supercontinuum laser power during the monochromator
operation. The ON/OFF illumination for the transient
photocurrent was chopped using an optical chopper system
5746 https://dx.doi.org/10.1021/acs.nanolett.0c01460
Nano Lett. 2020, 20, 5741−5748
Nano Letters pubs.acs.org/NanoLett
(300CD, Scitec Instruments). The rapid increase and decrease
in the transient photocurrent was measured by a low-noise
current preamplifier (SR570, SRS) using a data acquisition
(DAQ) system with a sampling rate of 500 KS/s (NI 6343 X
Series Data Acquisition, National Instruments).
■
ASSOCIATED CONTENT
*
sı Supporting Information
The Supporting Information is available free of charge at
https://pubs.acs.org/doi/10.1021/acs.nanolett.0c01460.
Device fabrication process; depletion layer calculation;
photoluminescence spectra of WSe2−MoS2, MoS2, and
WSe2; energy band diagram for the operation mecha-
nism of the device; photocurrent maps of photovoltaic
effect; temporal response of the device at the different
gate voltages; physical parameters for the calculation of
the photoconductive gain; and performance comparison
of photo transistors (PDF)
■
AUTHOR INFORMATION
Corresponding Author
Sung-Yool Choi − School of Electrical Engineering, Graphene/
2D Materials Research Center, Center for Advanced Materials
Discovery towards 3D Display, KAIST, Daejeon 34141,
Republic of Korea; orcid.org/0000-0002-0960-7146;
Email: sungyool.choi@kaist.ac.kr
Authors
Gwang Hyuk Shin − School of Electrical Engineering,
Graphene/2D Materials Research Center, Center for Advanced
Materials Discovery towards 3D Display, KAIST, Daejeon
34141, Republic of Korea
Cheolmin Park − School of Electrical Engineering, Graphene/
2D Materials Research Center, Center for Advanced Materials
Discovery towards 3D Display, KAIST, Daejeon 34141,
Republic of Korea
Khang June Lee − School of Electrical Engineering, Graphene/
2D Materials Research Center, Center for Advanced Materials
Discovery towards 3D Display, KAIST, Daejeon 34141,
Republic of Korea
Hyeok Jun Jin − School of Electrical Engineering, Graphene/2D
Materials Research Center, Center for Advanced Materials
Discovery towards 3D Display, KAIST, Daejeon 34141,
Republic of Korea
Complete contact information is available at:
https://pubs.acs.org/10.1021/acs.nanolett.0c01460
Author Contributions
† H. L.; Konstantatos, G. Hybrid 2D−0D MoS2−PbS Quantum Dot
These two authors contributed equally to this work.
Notes
The authors declare no competing financial interest.
■
ACKNOWLEDGMENTS
This work was supported by the National Research
Foundation of Korea (NRF) through the Creative Materials
Discovery Program (2016M3D1A1900035) and Basic Re-
search Program (2019R1A2C2009171).
■
REFERENCES
(1) Chow, P. C. Y.; Matsuhisa, N.; Zalar, P.; Koizumi, M.; Yokota,
T.; Someya, T. Dual-Gate Organic Phototransistor with High-Gain
and Linear Photoresponse. Nat. Commun. 2018, 9 (1), 4546.
5747
Letter
(2) Guo, F.; Yang, B.; Yuan, Y.; Xiao, Z.; Dong, Q.; Bi, Y.; Huang, J.
A Nanocomposite Ultraviolet Photodetector based on Interfacial
Trap-Controlled Charge Injection. Nat. Nanotechnol. 2012, 7 (12),
798−802.
(3) Pierre, A.; Gaikwad, A.; Arias, A. C. Charge-Integrating Organic
Heterojunction Phototransistors for Wide-Dynamic-Range Image
Sensors. Nat. Photonics 2017, 11 (3), 193−199.
(4) Park, S.; Kim, S. J.; Nam, J. H.; Pitner, G.; Lee, T. H.; Ayzner, A.
L.; Wang, H.; Fong, S. W.; Vosgueritchian, M.; Park, Y. J.;
Brongersma, M. L.; Bao, Z. Significant Enhancement of Infrared
Photodetector Sensitivity Using a Semiconducting Single-Walled
Carbon Nanotube/C60 Phototransistor. Adv. Mater. 2015, 27 (4),
759−765.
(5) Rim, Y. S.; Yang, Y.; Bae, S.-H.; Chen, H.; Li, C.; Goorsky, M. S.;
Yang, Y. Ultrahigh and Broad Spectral Photodetectivity of an
Organic−Inorganic Hybrid Phototransistor for Flexible Electronics.
Adv. Mater. 2015, 27 (43), 6885−6891.
(6) Wang, Q. H.; Kalantar-Zadeh, K.; Kis, A.; Coleman, J. N.;
Strano, M. S. Electronics and Optoelectronics of Two-Dimensional
Transition Metal Dichalcogenides. Nat. Nanotechnol. 2012, 7 (11),
699−712.
(7) Fiori, G.; Bonaccorso, F.; Iannaccone, G.; Palacios, T.;
Neumaier, D.; Seabaugh, A.; Banerjee, S. K.; Colombo, L. Electronics
based on Two-Dimensional Materials. Nat. Nanotechnol. 2014, 9 (10),
768−779.
(8) Xia, F.; Wang, H.; Xiao, D.; Dubey, M.; Ramasubramaniam, A.
Two-Dimensional Material Nanophotonics. Nat. Photonics 2014, 8
(12), 899−907.
(9) Castellanos-Gomez, A. Why all the fuss about 2D Semi-
conductors? Nat. Photonics 2016, 10 (4), 202−204.
(10) Radisavljevic, B.; Kis, A. Mobility Engineering and A Metal−
Insulator Transition in Monolayer MoS2. Nat. Mater. 2013, 12 (9),
815−820.
(11) Kim, S.; Konar, A.; Hwang, W.-S.; Lee, J. H.; Lee, J.; Yang, J.;
Jung, C.; Kim, H.; Yoo, J.-B.; Choi, J.-Y.; Jin, Y. W.; Lee, S. Y.; Jena,
D.; Choi, W.; Kim, K. High-Mobility and Low-Power Thin-Film
Transistors based on Multilayer MoS2 Crystals. Nat. Commun. 2012,
3 (1), 1011.
(12) Zhang, W.; Huang, J.-K.; Chen, C.-H.; Chang, Y.-H.; Cheng,
Y.-J.; Li, L.-J. High-Gain Phototransistors Based on a CVD
MoS2Monolayer. Adv. Mater. 2013, 25 (25), 3456−3461.
(13) Kufer, D.; Konstantatos, G. Highly Sensitive, Encapsulated
MoS2 Photodetector with Gate Controllable Gain and Speed. Nano
Lett. 2015, 15 (11), 7307−7313.
(14) Choi, W.; Cho, M. Y.; Konar, A.; Lee, J. H.; Cha, G.-B.; Hong,
S. C.; Kim, S.; Kim, J.; Jena, D.; Joo, J.; Kim, S. High-Detectivity
Multilayer MoS2 Phototransistors with Spectral Response from
Ultraviolet to Infrared. Adv. Mater. 2012, 24 (43), 5832−5836.
(15) Lee, H. S.; Min, S.-W.; Chang, Y.-G.; Park, M. K.; Nam, T.;
Kim, H.; Kim, J. H.; Ryu, S.; Im, S. MoS2 Nanosheet Phototransistors
with Thickness-Modulated Optical Energy Gap. Nano Lett. 2012, 12
(7), 3695−3700.
(16) Kufer, D.; Nikitskiy, I.; Lasanta, T.; Navickaite, G.; Koppens, F.
Photodetectors. Adv. Mater. 2015, 27 (1), 176−180.
(17) Huo, N.; Konstantatos, G. Ultrasensitive All-2D MoS2
Phototransistors Enabled by An Out-of-Plane MoS2 PN Homo-
junction. Nat. Commun. 2017, 8 (1), 572.
(18) Kim, S.-G.; Kim, S.-H.; Park, J.; Kim, G.-S.; Park, J.-H.;
Saraswat, K. C.; Kim, J.; Yu, H.-Y. Infrared Detectable MoS2
Phototransistor and Its Application to Artificial Multilevel Optic-
Neural Synapse. ACS Nano 2019, 13 (9), 10294−10300.
(19) Zhang, Q.; Bao, W.; Gong, A.; Gong, T.; Ma, D.; Wan, J.; Dai,
J.; Munday, J. N.; He, J.-H.; Hu, L.; Zhang, D. A Highly Sensitive,
Highly Transparent, Gel-Gated MoS2 Phototransistor on Biodegrad-
able Nanopaper. Nanoscale 2016, 8 (29), 14237−14242.
(20) Lopez-Sanchez, O.; Lembke, D.; Kayci, M.; Radenovic, A.; Kis,
A. Ultrasensitive Photodetectors based on Monolayer MoS2. Nat.
Nanotechnol. 2013, 8 (7), 497−501.
https://dx.doi.org/10.1021/acs.nanolett.0c01460
Nano Lett. 2020, 20, 5741−5748
Nano Letters pubs.acs.org/NanoLett Letter

(21) Wang, X.; Wang, P.; Wang, J.; Hu, W.; Zhou, X.; Guo, N.; (39) Xu, J.; Jia, J.; Lai, S.; Ju, J.; Lee, S. Tunneling Field Effect
Huang, H.; Sun, S.; Shen, H.; Lin, T.; Tang, M.; Liao, L.; Jiang, A.; Transistor Integrated with Black Phosphorus-MoS2 Junction and Ion
Sun, J.; Meng, X.; Chen, X.; Lu, W.; Chu, J. Ultrasensitive and Gel Dielectric. Appl. Phys. Lett. 2017, 110 (3), 033103.
Broadband MoS2 Photodetector Driven by Ferroelectrics. Adv. Mater. (40) Doan, M.-H.; Jin, Y.; Adhikari, S.; Lee, S.; Zhao, J.; Lim, S. C.;
2015, 27 (42), 6575−6581. Lee, Y. H. Charge Transport in MoS2/WSe2 van der Waals
(22) Yin, Z.; Li, H.; Li, H.; Jiang, L.; Shi, Y.; Sun, Y.; Lu, G.; Zhang, Heterostructure with Tunable Inversion Layer. ACS Nano 2017, 11
Q.; Chen, X.; Zhang, H. Single-Layer MoS2 Phototransistors. ACS (4), 3832−3840.
Nano 2012, 6 (1), 74−80. (41) Liu, X.; Qu, D.; Li, H.-M.; Moon, I.; Ahmed, F.; Kim, C.; Lee,
(23) Park, J.; Park, Y.; Yoo, G.; Heo, J. Bias-Dependent M.; Choi, Y.; Cho, J. H.; Hone, J. C.; Yoo, W. J. Modulation of
Photoresponsivity of Multi-Layer MoS2 Phototransistors. Nanoscale Quantum Tunneling via a Vertical Two-Dimensional Black
Res. Lett. 2017, 12 (1), 599. Phosphorus and Molybdenum Disulfide p−n Junction. ACS Nano
(24) Yoo, G.; Choi, S. L.; Park, S. J.; Lee, K.-T.; Lee, S.; Oh, M. S.; 2017, 11 (9), 9143−9150.
Heo, J.; Park, H. J. Flexible and Wavelength-Selective MoS2 (42) Li, H.; Ye, L.; Xu, J. High-Performance Broadband Floating-
Phototransistors with Monolithically Integrated Transmission Color Base Bipolar Phototransistor Based on WSe2/BP/MoS2 Hetero-
Filters. Sci. Rep. 2017, 7 (1), 40945. structure. ACS Photonics 2017, 4 (4), 823−829.
(25) Zhang, K.; Zhang, T.; Cheng, G.; Li, T.; Wang, S.; Wei, W.; (43) Deng, Y.; Luo, Z.; Conrad, N. J.; Liu, H.; Gong, Y.; Najmaei, S.;
Zhou, X.; Yu, W.; Sun, Y.; Wang, P.; Zhang, D.; Zeng, C.; Wang, X.; Ajayan, P. M.; Lou, J.; Xu, X.; Ye, P. D. Black Phosphorus−Monolayer
Hu, W.; Fan, H. J.; Shen, G.; Chen, X.; Duan, X.; Chang, K.; Dai, N. MoS2 van der Waals Heterojunction p−n Diode. ACS Nano 2014, 8
Interlayer Transition and Infrared Photodetection in Atomically Thin (8), 8292−8299.
Type-II MoTe2/MoS2 van der Waals Heterostructures. ACS Nano (44) Lee, C.-H.; Lee, G.-H.; van der Zande, A. M.; Chen, W.; Li, Y.;
2016, 10 (3), 3852−3858. Han, M.; Cui, X.; Arefe, G.; Nuckolls, C.; Heinz, T. F.; Guo, J.; Hone,
(26) Wang, F.; Wang, Z.; Xu, K.; Wang, F.; Wang, Q.; Huang, Y.; J.; Kim, P. Atomically Thin p−n Junctions with van der Waals
Yin, L.; He, J. Tunable GaTe-MoS2 van der Waals p−n Junctions Heterointerfaces. Nat. Nanotechnol. 2014, 9 (9), 676−681.
with Novel Optoelectronic Performance. Nano Lett. 2015, 15 (11), (45) Furchi, M. M.; Pospischil, A.; Libisch, F.; Burgdörfer, J.;
7558−7566. Mueller, T. Photovoltaic Effect in an Electrically Tunable van der
(27) Choi, M. S.; Qu, D.; Lee, D.; Liu, X.; Watanabe, K.; Taniguchi, Waals Heterojunction. Nano Lett. 2014, 14 (8), 4785−4791.
T.; Yoo, W. J. Lateral MoS2 p−n Junction Formed by Chemical (46) Mak, K. F.; Lee, C.; Hone, J.; Shan, J.; Heinz, T. F. Atomically
Doping for Use in High-Performance Optoelectronics. ACS Nano Thin MoS2: A New Direct-Gap Semiconductor. Phys. Rev. Lett. 2010,
2014, 8 (9), 9332−9340. 105 (13), 136805.
(28) Pak, J.; Lee, I.; Cho, K.; Kim, J.-K.; Jeong, H.; Hwang, W.-T.; (47) Moazzami, K.; Murphy, T. E.; Phillips, J. D.; Cheung, M. C. K.;
Ahn, G. H.; Kang, K.; Yu, W. J.; Javey, A.; Chung, S.; Lee, T. Intrinsic Cartwright, A. N. Sub-Bandgap Photoconductivity in ZnO Epilayers
Optoelectronic Characteristics of MoS2 Phototransistors via a Fully and Extraction of Trap Density Spectra. Semicond. Sci. Technol. 2006,
Transparent van der Waals Heterostructure. ACS Nano 2019, 13 (8), 21 (6), 717−723.
9638−9646.
(29) Lee, Y. T.; Kang, J.-H.; Kwak, K.; Ahn, J.; Choi, H. T.; Ju, B.-K.;
Shokouh, S. H.; Im, S.; Park, M.-C.; Hwang, D. K. High-Performance
2D MoS2 Phototransistor for Photo Logic Gate and Image Sensor.
ACS Photonics 2018, 5 (12), 4745−4750.
(30) Cui, X.; Lee, G.-H.; Kim, Y. D.; Arefe, G.; Huang, P. Y.; Lee,
C.-H.; Chenet, D. A.; Zhang, X.; Wang, L.; Ye, F.; Pizzocchero, F.;
Jessen, B. S.; Watanabe, K.; Taniguchi, T.; Muller, D. A.; Low, T.;
Kim, P.; Hone, J. Multi-Terminal Transport Measurements of MoS2
using a van der Waals Heterostructure Device Platform. Nat.
Nanotechnol. 2015, 10 (6), 534−540.
(31) Geim, A. K.; Grigorieva, I. V. Van der Waals Heterostructures.
Nature 2013, 499 (7459), 419−425.
(32) Jariwala, D.; Marks, T. J.; Hersam, M. C. Mixed-dimensional
van der Waals Heterostructures. Nat. Mater. 2017, 16 (2), 170−181.
(33) Wang, X.; Xia, F. Stacked 2D Materials Shed Light. Nat. Mater.
2015, 14 (3), 264−265.
(34) Novoselov, K. S.; Mishchenko, A.; Carvalho, A.; Castro Neto,
A. H. 2D Materials and van der Waals Heterostructures. Science 2016,
353 (6298), aac9439.
(35) Gong, Y.; Lin, J.; Wang, X.; Shi, G.; Lei, S.; Lin, Z.; Zou, X.; Ye,
G.; Vajtai, R.; Yakobson, B. I.; Terrones, H.; Terrones, M.; Tay, B. K.;
Lou, J.; Pantelides, S. T.; Liu, Z.; Zhou, W.; Ajayan, P. M. Vertical and
In-Plane Heterostructures from WS2/MoS2Monolayers. Nat. Mater.
2014, 13 (12), 1135−1142.
(36) Nourbakhsh, A.; Zubair, A.; Dresselhaus, M. S.; Palacios, T.
Transport Properties of a MoS2/WSe2 Heterojunction Transistor
and Its Potential for Application. Nano Lett. 2016, 16 (2), 1359−
1366.
(37) Roy, T.; Tosun, M.; Cao, X.; Fang, H.; Lien, D.-H.; Zhao, P.;
Chen, Y.-Z.; Chueh, Y.-L.; Guo, J.; Javey, A. Dual-Gated MoS2/WSe2
van der Waals Tunnel Diodes and Transistors. ACS Nano 2015, 9 (2),
2071−2079.
(38) Roy, T.; Tosun, M.; Hettick, M.; Ahn, G. H.; Hu, C.; Javey, A.
2D-2D Tunneling Field-Effect Transistors using WSe2/SnSe2
Heterostructures. Appl. Phys. Lett. 2016, 108 (8), 083111.

5748 https://dx.doi.org/10.1021/acs.nanolett.0c01460
Nano Lett. 2020, 20, 5741−5748