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Article

www.acsnano.org

Strain-Gated Field Effect Transistor of a MoS2−


ZnO 2D−1D Hybrid Structure
Libo Chen,†,§ Fei Xue,†,§ Xiaohui Li,† Xin Huang,† Longfei Wang,† Jinzong Kou,†
and Zhong Lin Wang*,†,‡

Beijing Institute of Nanoenergy and Nanosystems, Chinese Academy of Sciences, Beijing, 100083, China

School of Material Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
*
S Supporting Information

ABSTRACT: Two-dimensional (2D) molybdenum disulfide (MoS2) is an


exciting material due to its unique electrical, optical, and piezoelectric
properties. Owing to an intrinsic band gap of 1.2−1.9 eV, monolayer or a-few-
layer MoS2 is used for fabricating field effect transistors (FETs) with high
electron mobility and on/off ratio. However, the traditional FETs are
controlled by an externally supplied gate voltage, which may not be sensitive
enough to directly interface with a mechanical stimulus for applications in
electronic skin. Here we report a type of top-pressure/force-gated field effect
transistors (PGFETs) based on a hybrid structure of a 2D MoS2 flake and 1D
ZnO nanowire (NW) array. Once an external pressure is applied, the
piezoelectric polarization charges created at the tips of ZnO NWs grown on
MoS2 act as a gate voltage to tune/control the source−drain transport property
in MoS2. At a 6.25 MPa applied stimulus on a packaged device, the source−
drain current can be tuned for ∼25%, equivalent to the results of applying an extra −5 V back gate voltage. Another type of
PGFET with a dielectric layer (Al2O3) sandwiched between MoS2 and ZnO also shows consistent results. A theoretical
model is proposed to interpret the received data. This study sets the foundation for applying the 2D material-based FETs in
the field of artificial intelligence.
KEYWORDS: strain/pressure, field effect transistors, MoS2, ZnO, piezotronic effect

M oS2, as a member of the 2D transition-metal


dichalcogenide material system, has unique elec-
trical, optical, and piezoelectric properties1−10 and
can be exfoliated into monolayer or few-layer flakes.11−13 Each
2D MoS2 layer possesses three atomic layers of 6.5 Å thickness,
excellent choices to fabricate smart devices with functions of
sensitively detecting an external mechanical stimulus and
simultaneously converting this stimulus to electrical sig-
nals.21−25 Here we present a pressure-gated FET (PGFET)
using a hybrid structure of a 2D MoS2 flake and a 1D ZnO
where the molybdenum atom plane is sandwiched between two nanowire (NW) array.
planes of sulfur atoms with the covalently bonded S−Mo−S
atoms in a commonly found hexagonal-structured crystal.14 RESULTS AND DISCUSSION
Monolayer MoS2 is confirmed to have a direct intrinsic band Single- or few-layer MoS2 flakes were exfoliated from bulk
gap of ∼1.85 eV and will change to an indirect band gap of 1.2 MoS2 and directly attached on highly doped p-type silicon
eV with layers increased to bulk.14−16 Combined with a high- substrates covered with 300 nm thick SiO2, which is optimum
quality dielectric layer, monolayer or few-layer ultrathin MoS2 for optical detection of MoS2 flakes. Electrical contacts were
field effect transistors (FETs) have been demonstrated with patterned on MoS2 flakes using lithography followed by
high mobility (>200 cm2 V−1 s−1) and on/off ratio (∼108),1 successive deposition of Cr and Au. The precise location and
near-ideal subthreshold swing (∼70 mV per decade), and large region where the ZnO NW array would be grown at low
current saturation window.2,17 temperature were defined by electron beam lithography, which
FETs, as a basic component of modern electronics, are based guaranteed that ZnO NWs on the top of the MoS2 flake were
on a fundamental principle that the source−drain current is isolated from the source and drain electrodes (for more details
gated by an applied voltage tuning the channel width.18 A see Supplementary Figure 1a). A schematic diagram and the
silicon-based FET has to be integrated with a capacitor or a
piezoelectric layer in order to sense an externally applied Received: November 11, 2015
mechanical stimulus.19,20 Recently, piezoelectric semiconductor Accepted: December 22, 2015
materials, such as ZnO, GaN, and CdS, are reported as Published: December 22, 2015

© 2015 American Chemical Society 1546 DOI: 10.1021/acsnano.5b07121


ACS Nano 2016, 10, 1546−1551
ACS Nano Article

Figure 1. Device structure and characterization of ZnO NWs and MoS2 flake. (a) Schematic illustration of a FET based on a MoS2 and ZnO
heterostructure. Using electron beam lithography, a small gap between source and drain electrodes was created, in which the ZnO nanowires
were grown. (b) SEM images of the device before coating an epoxy layer for packaging. Inset: Enlarged side-view (left-hand) and top-view
(right-hand) of the synthesized ZnO NW array. Scale bar: 3 μm in the large image and 1 μm in the inset images. (c) Raman spectrum of the
MoS2 flake used in this device.

Figure 2. Response of the pressure-gated FET based on the MoS2−ZnO heterostructure (Dev. 1). (a) Equivalent electrical circuit of the
device. The heterostructure between the MoS2 flake and ZnO NWs is represented by a diode. The characterizations of back gate electrically
controlled FET: Ids−Vds output curves (b) and Ids−Vgs transfer curves (c). (d) Pressure’s modulation on the output curves of Dev. 1. The
piezopotential of the ZnO NWs induced by the external stimulus acts as a gate voltage. Inset: Quantitative characterization of pressure versus
drain current (Ids). (e) Relative change in source−drain current derived from (d). Ids0 represents the drain current without applied pressure.
Almost ∼25% drain current change is obtained at the point of ∼2.5 V drain voltage under the pressure of 6.25 MPa and gate voltage of −15 V.
(f) Pressure-dependent change in drain current occurs at a bias voltage of 0.5 V drain and 0 V gate. Right-hand inset: Change in drain current
plotted versus applied pressure, which shows that a linear variation of drain current versus pressure will reach saturation when the pressure is
more than 4 MPa. (g) Observed change in drain current by periodically applying pressure to the device at the same bias voltage in (f).

corresponding practical device image (Dev. 1) are shown in channel between the source and drain electrodes is about 7 μm,
Figure 1a and b. A layer of epoxy was used to encapsulate the among which the ZnO NWs were grown via solution chemistry
entire device to keep its stability, which of course increased the nearly perpendicularly to the substrate without contact with
strain required to generate the desired gating effect. The either electrode. This heterostructure of 2D MoS2-contacted
1547 DOI: 10.1021/acsnano.5b07121
ACS Nano 2016, 10, 1546−1551
ACS Nano Article

Figure 3. Response of the pressure-gated FET with an Al2O3 insulator layer sandwiched between MoS2 and ZnO (Dev. 2). (a and b) Schematic
cartoon graphs of the architecture of Dev. 2. The ZnO NW array and MoS2 flake are separated by a 20 nm ALD-deposited Al2O3 layer. (c)
SEM image of our practical device. Scale bar: 3 μm. Ids−Vds output (d) and Ids−Vgs transfer characteristics (e) of the electrically controlled
Dev. 2. (f) Response of the pressure-gated FET based on a MoS2−Al2O3−ZnO hybrid structure under different gate voltages. With the
pressure increasing, the drain current exhibits an increasing trend. (g) Pressure-dependent change in drain current at the drain voltage of 1 V
and gate voltage of 2 V. Bottom inset: Plot of ΔIds with an increase in applied pressure. A saturated region appears when the pressure is more
than 4 MPa.

1D ZnO NWs allows the piezopotential of the ZnO NWs, for all fabricated devices regardless of the number of MoS2
induced by the externally applied mechanical stimulus, to act as layers. We note that, compared with the MoS2 FETs, the
a gate to modulate the FET output. Before device fabrication, overall performance of the heterostructure FETs based on
Raman characterization is employed to identify the thickness of MoS2−ZnO was degraded by the solution process for
the MoS2 flakes (Supplementary Figure 2).26,27 The Raman synthesizing ZnO NWs (Supplementary Figure 4).
spectrum (Figure 1c) shows that the distance between the in- Then we characterized the pressure-controlled response of
plane E2g1 mode and out-of-plane A1g mode is 22 cm−1, which Dev. 1 as systematically interpreted in Figure 2d−g. From the
confirms that the MoS2 flake used for Dev. 1 was three layers.28 pressure-dependent output curves (Figure 2d), it is observed
The equivalent electrical circuit of Dev. 1 is illustrated in that increasing the pressure gives rise to a steadily decreasing
Figure 2a. We define the heterostructure of MoS2−ZnO as a drain current in spite of a different gate voltage. The inset
diode, whose turn-on voltage is positive. The electrical exhibits that the decreasing trend could reach saturation, as
characterization of the devices was performed at room demonstrated previously,22 with the pressure increased under
temperature using a shielded probe station and a semi- different drain bias voltages and gate step voltages. A relative
conductor parameter analyzer. The external pressure was change of drain current as shown in Figure 2e is defined as |ΔI/
applied by a digital force gauge (Supplementary Figure 3). Idso|, where Idso represents the drain current without applying
All measurements were carried out in the dark because visible pressure and ΔI is the change in current after applying pressure.
light can significantly increase the device’s drain current due to Notably, a maximum peak for about 25% occurs at ∼2.5 V
the photoelectrical effect of MoS2. We first characterized the when the external pressure is fixed at 6.25 MPa and the gate
back gate electrically controlled response of the MoS 2 voltage at −15 V, which is equivalent to the result of applying
heterostructure FET by applying a bias voltage to the drain an additional ∼−5 V back gate voltage. Figure 2f presents the
and step voltage to a highly doped p-type silicon substrate with pressure-dependent change in drain current under a drain
the source grounded as indicated in Figure 2a. The typical voltage of 0.5 V and gate voltage of 0 V. Externally applied
output and transfer characteristics are presented in Figure 2b pressure yields a piezopotential via ZnO NWs to modulate the
and c, respectively. The Ids−Vds output curves increase when output of the device, effectively acting as a back gate voltage. As
the gate voltage is increased owing to the free electron the graph at the right-hand side of Figure 2f indicates, the
accumulation in the MoS2 channel. This indicates that the change in drain current is almost linear to the applied pressure
semiconducting MoS2 used here is an n-type,2 which is the case below ∼4 MPa and then reaches a saturated region.
1548 DOI: 10.1021/acsnano.5b07121
ACS Nano 2016, 10, 1546−1551
ACS Nano Article

Figure 4. Schematic band diagrams to illustrate the underlying physical mechanism observed for the decreasing and increasing trends at an
applied pressure for the two types of devices. (a) Piezopotential distributions in a ZnO nanowire (35 nm in length and 4 nm in diameter)
under an axial force of 12 nN, simulated by a finite-element analysis method (COMSOL). (b) Energy bands of a MoS2−ZnO heterostructure
before (top) and after (bottom) applying a compressive force on ZnO NWs (Dev. 1). (c) Band diagrams of the MoS2−Al2O3−ZnO structure
before (top) and after (bottom) applying a pressure on ZnO (Dev. 2). See text for details.

Repeatability of the drain current variation at a periodically Finally, we fabricated a series of FETs to reveal the
applied pressure of 6.25 MPa is shown in Figure 2g, exhibiting a underlying physical mechanism observed for the decreasing
good reproducibility. and increasing trends in Dev. 1 and Dev. 2, respectively. Five
Next, we developed another type of PGFET with a dielectric devices with the structure of Dev. 1 and five with the structure
layer sandwiched between MoS2 flakes and ZnO NWs (Dev. 2), of Dev. 2 were tested, and all of them show consistent changes
which are schematically presented in Figure 3a and b. A 20 nm in source−drain current as presented above (Supplementary
thick layer of high-quality Al2O3 was deposited on the as- Figure 6). In this configuration, the transport characteristic
fabricated MoS2 FET using atomic layer deposition (Supple- change is attributed to two effects: a piezoresistance effect,
mentary Figure 1b), which serves as an effective gate oxide. The which emphasizes the strain-induced band gap change, and a
orderly ZnO NW array is synthesized at the top of the Al2O3 piezotronic effect, which is the strain-induced piezopotential
layer shown in Figure 3c, under the same condition as for Dev. modulation of the barrier height at the interface of the metal−
1. The typical back gate electrically controlled characteristics of semiconductor and p−n junctions.22,29 To find out which
Dev. 2 are displayed in Figure 3d and e, respectively. The Ids− dominates the devices, control experiments were conducted on
Vds transport exhibits linear behavior at low drain voltage and the MoS2 flake FET without ZnO NWs on the top
excellent current saturation at high drain voltage, which is a (Supplementary Figure 4), which confirms that the piezore-
critical feature for both logic and analog circuits. When an sistance effect and the piezotronic effect in the MoS2 flake
external mechanical stimulus is applied, the piezopotential of cannot produce the change in drain current for the hybridized
structure. Therefore, the observed change in transport current
the ZnO NWs serves as a gate voltage that controls the channel
for Dev. 1 and Dev. 2 when a pressure is applied can be caused
conductance. Figure 3f and g display the pressure-dependent
only by the piezotronic effect of ZnO NWs on the MoS2 flake.
output characteristics of Dev. 2. It is worth mentioning that the
According to the piezotronic theory,30 we proposed a
source−drain current gradually increases with the increasing of schematic band diagram to interpret the stated increasing and
applied pressure, which is just opposite that of Dev. 1. The decreasing trends in Dev. 1 and Dev. 2 as shown in Figure 4.
vertical structure of MoS2−Al2O3−ZnO forms a typical The piezopotential distribution in a ZnO NW under an applied
capacitance like a traditional metal-oxide−semiconductor force is simulated by a finite-element analysis method
(MOS) structure. This significant feature distinguishes it from (COMSOL). When a force is applied on the nanowire, the
the FET based on a MoS2−ZnO heterostructure and results in superposition of the electric dipole moment along the c-axis
their exactly opposite response to external pressure, which will generates negative and positive piezoelectric polarization
be discussed in detail later. The distinct pressure-controlled charges (piezopotential) along the positive and negative c-
change in drain current of Dev. 2 is also clearly illustrated in the axis, respectively, as indicated in Figure 4a. The as-synthesized
top graph of Figure 3g, where the variation of output current ZnO NWs and the exfoliated MoS2 flakes are all naturally n-
(ΔIds) is plotted as a function of time for different applied type.2,21 An n−n homotype heterojunction forms at the
pressure to the local ZnO NWs. The gate voltage and drain interface of these two semiconducting materials.31 Due to the
voltage were fixed at 2 and 1 V, respectively, to achieve a large different work function and electron affinity between ZnO and
current variation (Supplementary Figure 5). The bottom graph MoS2 (Supplementary Figure 7), electrons in the ZnO NWs
shows quantitative characterization of the variation trend of may diffuse into the MoS2 flakes at the junction area to balance
pressure versus the change in drain current, where a saturated the different Fermi levels as for Dev. 1, yielding a positively
region also occurs when the pressure is more than ∼4 MPa. charged carrier (electron) depletion region on the ZnO side
1549 DOI: 10.1021/acsnano.5b07121
ACS Nano 2016, 10, 1546−1551
ACS Nano Article

and a negatively charged carrier accumulation region on the ASSOCIATED CONTENT


MoS2 side.18 Under an equilibrium state, a barrier at the *
S Supporting Information
interface as shown in Figure 4b forms, which is of great The Supporting Information is available free of charge on the
significance to the modulation of the piezopotential on the ACS Publications website at DOI: 10.1021/acsnano.5b07121.
channel current. Once pressure is applied on the ZnO NWs,
Device fabrication (Figure S1), Raman spectrum (Figure
the induced positive piezoelectric polarization charges in the
S2), optical graph of the testing platform (Figure S3),
depletion region lower the local barrier height,30 leading to a
pressure’s influence on the performance of a MoS2
redistribution of carriers at the junction region. Specifically, the
transistor without any hybrid structure (Figure S4),
mobile negative electrons in the MoS2 conducting channel are drain current change under different pressures and gate
attracted across the lowered barrier to screen the positive voltages as for Dev. 2 (Figure S5), histograms of change
polarization charges on the ZnO side (Figure 4b); the reduced in drain current for two group devices at 2 MPa (Figure
carrier concentration in MoS2 decreases the drain current, as S6), electron affinity, work function, and band gaps of
observed in Figure 2d. MoS2 and ZnO used in the energy band diagrams
Band diagrams of MoS2−Al2O3−ZnO before (top) and after (Figure S7) (PDF)
(bottom) applying an external pressure on Dev. 2 are illustrated
in Figure 4c. Once a pressure is applied, the positive
AUTHOR INFORMATION
piezoelectric polarization charges are generated at the Al2O3−
ZnO interface and electrostatically induce mobile electrons in Corresponding Author
the MoS2 channel, similar to the case of traditional FETs gated *E-mail: zhong.wang@mse.gatech.edu.
by a back or top gate voltage. With increasing applied pressure, Author Contributions
§
more free electrons are accumulated at the interface of MoS2− L. Chen and F. Xue contributed equally.
Al2O3; accordingly the local carrier density is increased in the Notes
MoS2 channel,18 which yields an increase in source−drain The authors declare no competing financial interest.
current as indicated in Figure 3f and e. In brief, the positive
piezoelectric charges in ZnO NWs accumulate mobile electrons ACKNOWLEDGMENTS
in the MoS2 channel by electrostatic induction in the structure
We thank Dr. W. Liu, Dr. C. Zhang, Y. Zhou, and J. Liu for
of MoS2−Al2O3−ZnO, while deplete free electrons from the
helpful discussions. This research was supported by the
MoS2 channel in the structure of MoS2−ZnO. “Thousands Talents” program for pioneer researcher and his
innovation team, China, National Natural Science Foundation
CONCLUSIONS of China (Grant No. 51432005), and Beijing City Committee
In conclusion, we have demonstrated external pressure-gated of science and technology projects (Z131100006013004,
MoS2 FETs, in which a few-layer MoS2 flake acts as a Z131100006013005).
conductive channel and piezoelectric ZnO NWs act as a gate
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1551 DOI: 10.1021/acsnano.5b07121


ACS Nano 2016, 10, 1546−1551

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