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Das Et Al 2012 High Performance Multilayer Mos2 Transistors With Scandium Contacts

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Das Et Al 2012 High Performance Multilayer Mos2 Transistors With Scandium Contacts

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Soumya Maiti
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Letter

pubs.acs.org/NanoLett

High Performance Multilayer MoS2 Transistors with Scandium


Contacts
Saptarshi Das,* Hong-Yan Chen, Ashish Verma Penumatcha, and Joerg Appenzeller
Birck Nanotechnology Center & Department of ECE, Purdue University, West Lafayette, Indiana, United States
*
S Supporting Information

ABSTRACT: While there has been growing interest in two-


dimensional (2-D) crystals other than graphene, evaluating
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their potential usefulness for electronic applications is still in its


infancy due to the lack of a complete picture of their
performance potential. The focus of this article is on contacts.
We demonstrate that through a proper understanding and
design of source/drain contacts and the right choice of number
of MoS2 layers the excellent intrinsic properties of this 2-D
material can be harvested. Using scandium contacts on 10-nm-
thick exfoliated MoS2 flakes that are covered by a 15 nm Al2O3 film, high effective mobilities of 700 cm2/(V s) are achieved at
room temperature. This breakthrough is largely attributed to the fact that we succeeded in eliminating contact resistance effects
that limited the device performance in the past unrecognized. In fact, the apparent linear dependence of current on drain voltage
had mislead researchers to believe that a truly Ohmic contact had already been achieved, a misconception that we also elucidate
in the present article.
KEYWORDS: 2-d semiconductor, layered dichalcogenide, MoS2, field-effect transistor (FET), contact, mobility

L ow-dimensional materials in general and two-dimensional


(2-D) layered materials in particular are interesting not
only because they provide access to novel physical phenomena,
on evaluating and solving interface problems between the gate
dielectric and the 2-D semiconducting channel material to
obtain ultimate gate control,23,24 much less attention has been
but also because their unique electrical, optical, mechanical, and paid to the metal/semiconductor contact interface at the source
chemical properties make them attractive from a technological and drain end.
standpoint. Graphene, hexagonal boron nitride (h-BN), and In this Letter, we present a thorough experimental study of
more recently 2-D nanostructures of Bi2Se3 and Bi2Te3 contacts to MoS2 using in particular low work function metals
(topological insulator materials)1−5 are considered as promising like scandium (ΦM = 3.5 eV) and titanium (ΦM = 4.3 eV) to
candidates for various future nanoelectronics applications. shine some light on the impact of Schottky barriers on the
Another class of 2-D materials that is receiving an increasing carrier transport in MoS2 FETs. Our study is complemented by
amount of scientific attention, is the rich family of transition comparing the results obtained with large work function metals
metal dichalcogenides comprised of MoS2, WS2, WSe2, and like nickel (ΦM = 5.0 eV) and platinum (ΦM = 5.9 eV).
many more.6−12 While graphene shows the highest reported Recently a number of articles8,15,25,26 have utilized large work
mobility in excess of 100 000 cm2/(V s)13 within this family, function metals and yet reported excellent n-type contact
the absence of an energy gap in the electronic band structure of formation and electron injection without emphasizing the fact
graphene paves the way for the exploration of semiconducting that this experimental observation is rather peculiar.27 From a
2D materials like MoS214,15 and others. detailed temperature-dependent study that considers both
MoS2 is a semiconductor with an indirect bandgap of 1.2 eV thermionic emissions over the Schottky barrier as well as
(single-layer MoS2 shows a direct bandgap of 1.8 eV, and thermally assisted tunneling through the same, we have
bilayer MoS2 exhibits an indirect bandgap of 1.3 eV), an extracted the Schottky barrier height for the various metal
electron affinity of 4.0 eV16,17 and a maximum reported electrodes and found ∼230 meV for platinum, ∼150 meV for
mobility of 517 cm2/(V s)17 Single and multilayer MoS2 field- nickel, ∼50 meV for titanium, and ∼30 meV for scandium. Our
effect transistors (FETs) with on/off-current ratios as high as experiments provide unambiguous evidence that the MoS2-to-
108 and steep subthreshold swing (74 mV/decade) have metal interface is strongly impacted by Fermi level pinning
already been demonstrated in a top-gated transistor architec- close to the conduction band of the MoS2 similar to the case of
ture.8,18−20 Moreover, initial studies also indicate that MoS2 many III−V materials. While earlier reports had claimed that
may be useful for sensing and energy-harvesting applica-
tions.21,22 However, one of the major performance-limiting Received: September 26, 2012
factors for any low-dimensional material in general and 2-D Revised: November 29, 2012
materials in particular is the interface. While the focus has been Published: December 14, 2012

© 2012 American Chemical Society 100 dx.doi.org/10.1021/nl303583v | Nano Lett. 2013, 13, 100−105
Nano Letters Letter

gold (ΦM = 5.4 eV)-to-MoS2 contacts are Ohmic,8,15,25 our lithographic techniques were employed to pattern the source/
results clearly indicate the existence of Schottky barriers for drain contacts, and electron beam evaporation was used to
large work function metals like Ni and Pt. deposit the desired metal contacts (Sc, Ti, Ni, and Pt). The
We have also evaluated the field effect mobility of multilayer channel length for all of the devices is 5 μm, and the flake
MoS2 flakes for different metal contacts and different flake thicknesses range between 2 and 12 nm (3−18 mono layers).
thicknesses using a back-gated transistor geometry. As The deposited source/drain contact film thickness is 50 nm for
expected, the extracted mobility values were strongly depend- Ti, Ni, and Pt while to avoid damaging of the contacts in case of
ent on the metal-to-MoS2 contact interface; that is, the intrinsic scandium required a 30 nm Sc/20 nm Ni stack.
mobility is masked easily by the presence of the aforementioned Figure 2a shows the expected line-up of the metal Fermi level
Schottky barrier at the source and drain contacts. We have also with the electronic bands of MoS2 if only the difference of the
observed a nonmonotonic trend in the intrinsic field effect
mobility of MoS2 as a function of the MoS2 layer thickness. To
describe our experimental findings we have employed a model
including Thomas−Fermi charge screening and interlayer
coupling. The highest mobility values were obtained for a
finite layer thickness of around 10 nm. In this case the extracted
mobility values are 21, 90, 125, and 184 cm2/(V s) for Pt, Ni,
Ti ,and Sc contacts, respectively, clearly indicating that
improving the contact quality is essential to harvest the
intrinsic material properties.
A significant enhancement in the field effect mobility up to
700 cm2/(V s) is achieved by covering the top of the back-
gated MoS2 transistor with a thin layer of 15-nm-thick Al2O3.
While the mobility we find is substantially higher than
previously reported, the effect itself had been also observed
by other groups.8,10,12
Extraction of Schottky Barrier Height. Single-layer MoS2
consists of a stack of three hexagonally packed atomic layers of
sulfur−molybdenum−sulfur with strong intralayer covalent
bonding.16,17 In contrast, bulk MoS2 is a stack of single layers,
held together by weak van der Waals interlayer interaction and,
therefore, allows for micromechanical exfoliation of mono or Figure 2. (a) Expected (not correct) line-up of metal Fermi level with
few layerssimilar to the fabrication of graphene from the electronic bands of MoS2 flake if only the difference of the electron
affinity of MoS2 and the work function of the corresponding metal is
graphite. Figure 1a,b shows atomic force microscopy (AFM) considered. (b) The cartoon of expected transfer characteristics based
and optical images of a 3 nm (4 monolayer) thick MoS2 flake, on part a. (c) Transfer characteristics of back-gated 6-nm-thick MoS2
exfoliated using standard scotch tape technique on 100 nm transistor with Sc, Ti, Ni, and Pt metal contacts. The inset shows the
silicon dioxide (SiO2) substrate with underlying highly doped actual line-up based on the experimental data.
silicon. Figure 1c,d shows a 3-D sketch and an scanning
electron microscopy (SEM) image of a prototype back-gated
MoS2 transistor used for our contact study. Standard electron affinity of MoS2 and the work function of the
corresponding metal is considered. Electron injection should
occur for Sc and Ti, while Ni and Pt are expected to provide
access to the valence band and should thus enable hole
injection. Figure 2b illustrates the expected device character-
istics qualitatively under this assumption. On the other hand
Figure 2c shows the experimental transfer characteristics of
back gated MoS2 transistors with Sc, Ti, Ni, and Pt metal
contacts after adjusting for the threshold voltage shift. The
threshold voltages for Sc, Ti, Ni, and Pt contact devices were
found to be on average (sampled over 4−5 devices) −6.0, −1.0,
1.5, and 4.0 V, respectively. Threshold voltages are defined by
the deviation of the IDS versus VGS characteristics from their
exponential behavior in the subthreshold regime. Note that the
trend in the values of the threshold voltages is consistent with
the observed trend in on-currents.28 Interestingly, all of the
metal contacts exhibit n-type FET characteristics, which
indicate that the Fermi levels for all of these metals line-up
close to the conduction band edge of MoS2 as shown in the
inset of Figure 2c. Also, there is a clear trend of decreasing on-
state performance, that is, decreasing on-current for positive
Figure 1. (a) AFM image and (b) AFM height profile of a 3 nm thin VGS−VTH from Sc to Pt, suggesting a change in the charge
MoS2 flake. (c) SEM image and (d) 3-D cartoon of a prototype back- injection properties of the various contact metals. As will be
gated MoS2 transistor used for the study. discussed below these findings are consistent with Schottky
101 dx.doi.org/10.1021/nl303583v | Nano Lett. 2013, 13, 100−105
Nano Letters Letter

Figure 3. (a) Experimental transfer characteristics of a back-gated MoS2 transistor with Ni contacts at different operating temperatures. The insets
represent the energy band diagrams corresponding to the applied gate biases in three distinct regions: below flat band, below threshold, and above
threshold. (b) Arrhenius-type plot constructed using part a at different gate voltages and (c) extracted effective barrier height (ΦB) as a function of
applied gate voltages for Ni contact devices. (d) Extracted true Schottky barrier height ΦSB for different work function metals like Sc, Ti, Ni, and Pt.
The dotted line is a guide to the eyes.

barriers of varying heights formed at the metal-to-channel device, A is the Richardson’s constant, kB is the Boltzmann
interface, and a detailed temperature-dependent study has been constant, q is the electronic charge, T is the temperature, and
used to quantitatively analyze those barriers. VDS is the source to drain bias. VFB can now be readily
As described in greater detail in ref 29, tunneling through determined from ΦB (at the source-to-channel interface) as a
Schottky barrier at the source-to-channel interface is not only function of gate voltage. Figure 3c shows our findings for Ni
limiting the charge injection in the device on-state but also electrodes. For sufficiently negative gate voltages the effective
plays a critical role when evaluating the device off-state in the barrier height extracted from Figure 3b linearly responds to the
subthreshold region of the transistor. In fact it is the thermally gate voltage VGS (also see the Supporting Information). This is
assisted tunneling that impacts the inverse subthreshold slope a result of the fact that only Ithermionic determines the current
in Schottky barrier devices in general.30 The band bending flow through the device. It is when ΦB deviates from this linear
diagrams in Figure 3a illustrate the contributions of thermionic trend when Itunneling becomes relevant and VFB is reached. Note
emission current component (Ithermionic) and the thermally that the threshold voltage VTH that defines the device on-state
assisted tunneling current component (Itunneling) under different is larger than VFB. From Figure 3c, a true Schottky barrier
gate voltage conditions. Figure 3a shows the change in current height of 150 meV is extracted. Figure 3c also illustrates how
through the device with the gate voltage for different the wrong choice of gate voltageone that is larger than VFB
temperatures that are used to create the Arrhenius plot in can easily result in the extraction of a barrier height that is too
Figure 3b. When evaluating the current flow through the device small since thermally assisted tunneling adds another current
as a function of temperature, both contributionsIthermionic and component that is not included in the standard thermal
Itunnelingneed to be considered. The band diagrams also emission theory. It is this additional tunneling current that is
illustrate that the tunneling current can only be ignored when responsible for a perceived “Ohmic contact” at the interface
the gate voltage is below the flat band voltage VFB. If one can even for substantial Schottky barrier heights. The key is that an
identify VFB, the Arrhenius plot for this gate voltage will reveal ultrathin channel like MoS2 will always give rise to a short
the true Schottky barrier height ΦSB.31 To do so, the slope of tunneling distance and thus substantial tunneling currents as
the curves in Figure 3b in the high-temperature region is has been discussed in greater detail previously.32,33
analyzed assuming conventional thermionic emission theory. Figure 3d shows the extracted Schottky barrier heights for
Using the equation IDS = AT2 exp((qϕB)/(kBT)[1 − exp- the different metals used for our contact study as a function of
((qVDS)/(kBT))], the effective Schottky barrier height is their corresponding work functions. We find Schottky barrier
extracted. In this equation IDS is the current through the heights of 230, 150, 50, and 30 meV for Pt, Ni, Ti, and Sc,
102 dx.doi.org/10.1021/nl303583v | Nano Lett. 2013, 13, 100−105
Nano Letters Letter

respectively. In total more than 4−5 devices were characterized to drain bias (VDS) for low VDS values which is consistent with
per metal contact type under investigation. The extracted slope the fact that Pt exhibits the largest Schottky barrier height of
dΦSB/ dΦM of around 0.1 (note that this number is 230 meV. The current through Ni contacted devices, however,
approximately 0.27 in the case of silicon34) indicates that shows a linear dependence on VDS despite the presence of a
different from previous assumptions strong pinning at the sizable Schottky barrier of 150 meV at the Ni−MoS2 interface.
metal/MoS2 interface determines the line-up between the metal As discussed above, thermally assisted tunneling is responsible
Fermi level and the conduction band of MoS2. It also explains for this finite temperature effect, and consequently a linear
why only n-type characteristics are obtained in all reported relationship between current and drain voltage does not
cases27 even if large work function metals had been used. Note necessarily indicate an Ohmic contact.33 The increasing
that if the chemical reactivity, deposition-induced mechanical magnitude of the current from 0.1 to 0.7 to 1.0 to 4.8 μA/
deformation, or wettability of the metals was to influence the μm at a VDS of 1 V for Pt, Ni, Ti, and Sc contacted devices,
Schottky barrier height analysis significantly, the linear trend in respectively, is consistent with the fact that smaller Schottky
Figure 3d would be obscured. barrier heights at the metal-to-MoS2 interface result in better
Impact of Metal Contact. Next we turn our attention to carrier injection and hence smaller contact resistance values.
the impact of the Schottky barrier heights on the device Figure 4 also shows the transfer characteristics of 10-nm-
characteristics. The inset of Figure 4 shows the output thick MoS2 transistors with Sc, Ti, Ni, and Pt metal contacts for
VDS = 0.2 V at room temperature. The transconductance gm
(defined as gm = dIDS/dVGS) normalized by the width (gm/W)
shows a monotonic increase from 0.03, 0.14, 0.20 to 0.28 μS/
μm from Pt, Ni, Ti to Sc contacted devices. Field effect mobility
values of the ∼10 nm MoS2 flakes were extracted using the
conventional equation of gm = μnCOX(W/L)VDS at low VDS =
0.2 V (where μn is the field effect mobility and W and L are the
channel width and the channel length, respectively, COX = εOX/
dOX, where εOX is the dielectric constant and dOX is the
thickness of the gate oxide, dOX = 100 nm and for SiO2, εOX = 3
× 10−11, which gives COX ∼ 3 × 10−4 F/m2, and finally L ∼ 5
μm). The extracted effective field-effect mobility values were
found to be 21, 36, 125, and 184 cm2/(V s) for Pt, Ni, Ti, and
Sc contacted devices respectively, clearly highlighting how even
Figure 4. Transfer characteristics of 10 nm thin MoS2 back-gated small Schottky barriers can impact the mobility extraction
transistors with Sc, Ti, Ni, and Pt metal contacts at 300 K for VDS = 0.2
V. The inset shows the output characteristics of the corresponding significantly. Note that the maximum values of gm were used to
devices for a gate voltage overdrive of 4.0−5.0 V. extract the mobility values. The above findings clearly indicate
the importance of proper contact formation to harvest the
intrinsic properties of novel nano materials and explain the
characteristics of a back-gated ∼10-nm-thick MoS2 transistors extremely high mobility values reported below by the use of Sc
at 300 K for different metal contacts for the same gate voltage contacts. Also note that the mobility values extracted by
overdrive (VGS − VTH = 4 V) which corresponds to a carrier Radisavljevic et al.,8 for monolayer MoS2 and Wang et al.,12 for
concentration of ∼1.4 × 1012/cm2. The current through the Pt bilayer MoS2 using a back-gated device geometry are similar to
contact device shows an exponential dependence on the source ours prior to the deposition of a high-k dielectric layer and are

Figure 5. (a) Transfer characteristics of 20, 10, 6, 4, and 2 nm thick MoS2 field effect transistor with Sc as the source/drain contacts at room
temperature for VDS = 0.2 V. The inset shows the output characteristics for the same flakes for a gate overdrive voltage of 2 V. (b) The extracted
effective field effect mobility as a function of the MoS2 layer thickness. The dotted line is a fit to the experimental data using a model (inset) that
includes Thomas−Fermi screening with λ = 3.0 nm and interlayer conductivity with σint = 1 mS. The solid line is the simulated field effect mobility
without any interlayer resistance.

103 dx.doi.org/10.1021/nl303583v | Nano Lett. 2013, 13, 100−105


Nano Letters Letter

10 and 15 cm2/(V s), respectively, using Au and Ti/Au


contacts. This is consistent with our findings since Au is a high
work function metal (ΦM = 5.6 eV) and mono and bilayer
flakes have larger bandgaps that translate into even higher
Schottky barrier heights as reported here. To emphasize our
main finding again: the extracted mobility values for fully gated
metal contacted MoS2 FETs do not reflect the intrinsic mobility
of MoS2 unless highly transmissive contacts as scandium are
used.35
Ideal Layer Thickness. Back-gated MoS2 FETs with Sc as
the source and the drain contacts were fabricated using flake
thicknesses ranging from 2 to 70 nm. Figure 5a shows the
transfer and output characteristics (inset) of 2, 4, 6, 10, and 20
nm thick MoS2 FETs. The extracted room temperature field- Figure 6. Output characteristics of a high-performance MoS2 transistor
effect mobility values were found to depend strongly on the exhibiting extremely high mobility, saturation current density, and
transconductance for different gate overdrive voltages with 15 nm of
flake thickness in a nonmonotonic fashion as shown in Figure high-k dielectric (Al2O3). The inset shows transfer characteristics of
5b. This nonmonotonic trend suggests that, to harvest the the same device for different drain bias values.
maximum potential of MoS2 for high performance device
applications, a layer thickness in the range of 6−12 nm would
be ideal. The nonmonotonic trend can be readily explained consequence of the use of low Schottky barrier scandium
within the extension of a resistor network model (see inset of contacts and the suppression of substrate effects through the
Figure 5b) that we successfully employed before to describe use of a sufficiently thick MoS2 flake. A saturation current
transport in multilayer graphene devices.36 The key is that density of 240 μA/μm for a carrier density of ∼2.8 × 1012/cm2
metal source/drain contacts are connected only directly to the and a transconductance of 4.7 μS/μm at VDS = 1.0 V are
top MoS2 layer, while access to lower layers involves additional obtained for a channel length of 5 μm. Both values are higher
interlayer resistors (σint is the interlayer conductivity). Gating than previously reported data when considering the scaling
on the other hand impacts the lowest layers most, and charge aspects of FETs.12,39
screening results in a decreasing number of charges for top Conclusion. In conclusion, we have performed a thorough
MoS2 layers. For small layer thicknesses the absence of experimental study to determine the ideal metal contact for the
sufficient screening of the substrate impact results in a lower evaluation of intrinsic transport properties of MoS2 thin flake
mobility value than observed in bulk MoS2.37 For large layer field effect transistors. Our findings indicate that the metal-to-
thicknesses it is the finite interlayer conductivity σint that results MoS2 interface is strongly impacted by Fermi level pinning
in an effectively (not intrinsically) lower total mobility of the close to the conduction band of MoS2. Lower work function
system (as the Schottky barrier in case of Pt resulted in a lower metals like Sc have been employed to form improved contacts
effective mobility). The combination of these two components with thin MoS2 flakes, resulting in high carrier injection and
gives rise to a maximum mobility value for a finite layer lower contact resistances. We have observed a nonmonotonic
thickness. Our two-parameter model can be used to fit the trend in the effective field effect mobility of MoS2 flakes as a
experimental data well if we assume a Thomas−Fermi function of the layer thickness which can be modeled using a
screening length of λTF ∼ 3 nm and an interlayer conductivity resistor network and considering proper screening between
of 1 mS (see dotted curve in Figure 5b). Note that the individual layers. The intrinsic field-effect mobility of a 10-nm-
screening length is about 5 times larger than in the case of thick multilayer MoS2 flake was found to be as high as 184
multilayer graphene while the interlayer conductivity is about 8 cm2/(V s) and can be significantly boosted up to 700 cm2/(V
times smaller. Mobility plots similar to the one shown above are s) using a high-k dielectric environment. Record high saturation
observed for all metal contacts providing further evidence of current densities of 240 μA/μm for relatively low carrier
the applicability of the proposed resistor network. In general, concentrations of ∼2.8 × 1012/cm2 and record high trans-
the use of a finite number of MoS2 layers is beneficial since the conductance values of 4.7 μS/μm were measured providing
impact of the substrate on the device performance can be encouraging news about the usefulness of MoS2 for high-
performance electronics applications.


eliminated.
High-k for High Performance. Finally, to prove that the
above-reported mobility values are on par or even exceed ASSOCIATED CONTENT
previously reported experimental data, we followed an approach *
S Supporting Information

reported before that has shown to result in a substantial Extraction of Schottky barrier height: Sc, Ti, Ni, and Pt contact.
improvement in mobility after atomic layer deposition (ALD) This material is available free of charge via the Internet at
of high-k materials onto MoS2.8,11,12,18 We have combined this http://pubs.acs.org.
treatment with our findings about the ideal contact and layer
thickness from above by depositing 15 nm of Al2O3 on top of
our back-gated transistors. Figure 6 shows the measured output
■ AUTHOR INFORMATION
Notes
The authors declare no competing financial interest.


and transfer characteristics of a 10 nm MoS2 FET with
scandium contacts and ALD layer. The effective field-effect
mobility of the MoS2 flake extracted assuming a parallel plate ACKNOWLEDGMENTS
capacitor arrangement (ignoring any possible impact of fringing We would like to acknowledge Dave Lubelski for helping with
fields and the top dielectric) is increased by a factor of 3.8, from the Sc deposition and Ali Razavieh for ALD deposition. This
184 to 700 cm2/(V s). As mentioned above, this high value is a work was supported by the Nanotechnology Research Initiative
104 dx.doi.org/10.1021/nl303583v | Nano Lett. 2013, 13, 100−105
Nano Letters Letter

(NRI) through a supplement to the Network for Computa- (21) Eda, G.; Yamaguchi, H.; Voiry, D.; Fujita, T.; Chen, M.;
tional Nanotechnology (NCN), which is supported by National Chhowalla, M. Photoluminescence from Chemically Exfoliated MoS2.
Science Foundation (NSF) under grant no. EEC-0634750. Nano Lett. 2011, 11, 5111−16.


(22) Li, H.; et al. Fabrication of Single- and Multilayer MoS2 Film-
Based Field-Effect Transistors for Sensing NO at Room Temperature.
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