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Supporting Materials
Growth of Large-Area and Highly Crystalline
MoS2 Thin Layers on Insulating Substrates
By Keng-Ku Liu#, Wenjing Zhang#, Yi-Hsien Lee, Yu-Chuan Lin, Mu-Tung
Chang$,Ching-Yuan Su%, Chia-Seng Chang$, Hai Li@,Yumeng Shi, Hua Zhang@,
Chao-Sung Lai% and Lain-Jong Li&*

Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei, 10617, Taiwan

Institute of Physics, Academia Sinica, Taipei, 11529, Taiwan

Department of Electronic Engineering, Chang Gung University, Tao-Yuan 333,


Taiwan

School of Materials Science and Engineering, Nanyang Technological University,


Singapore.

&

Department of Photonics, National Chiao Tung University, HsinChu 300, Taiwan.

Department of Electrical Engineering and Computer Sciences, Massachusetts Institute


of Technology, Cambridge, Massachusetts 02139, USA
To whom correspondence should be addressed: (L. J. Li) lanceli@gate.sinica.edu.tw

Methods and Materials:


Transfer MoS2 onto fresh SiO2/Si substrates:
To transfer the as-grown MoS2 onto the fresh SiO2(300 nm)/Si substrate, the MoS2 was
coated with a layer of PMMA (Micro Chem. 950K A4) by spin-coating (step1: 500 rpm

for 10 sec; step 2: 3000 rpm for 60sec), followed by baking at 100oC for 10 min. After
that, the PMMA-caped MoS2 was then put into the NaOH (2M) solution at 100 oC for
30min. The PMMA-caped MoS2 film was transferred to a deionized(DI) water to dilute
and remove the etchant and residues. A fresh SiO2/Si substrate was then used to fish the
PMMA-caped MoS2 film, followed by drying on a hot-plate (100oC for 10 min). The
PMMA was removed by acetone, isopropyl alcohol (IPA) and then DI water. After that,
chloroform was used to further clean the MoS2 surfaces.
Characterizations:
The AFM images were performed in a Veeco Dimension-Icon system. The scanning
rate is 0.976 Hz with the 512 scanning lines. Raman spectra were collected in a NTMDT confocal Raman microscopic system (exciting laser wavelength 473 nm and laser
spot-size is of ~ 0.5 m). The Si peak at 520 cm-1 was used as reference for
wavenumber calibration in Raman characterization. The photoluminescence (PL)
measurements were performed with excitation from a solid-state laser with a power of
500 W at a wavelength of 473 nm. The laser radiation was focused onto the MoS2
sheets with a spot-size around 0.5m. Data collection time of PL was 1s for MoS2
sheets. The atomic structure of MoS2 sheets was characterization by a JEOL-2010F
TEM with accelerating voltage of 200k eV. Chemical configurations were determined
by X-ray photoelectron spectroscope (XPS, Phi V6000), performed with an Mg K Xray source on the samples. The energy calibrations were made against the C 1s peak to
eliminate the charging of the sample during analysis. The crystal structure and the
crystallinity were characterized by in-plan and glazing-incidence-angle (GIA) X-ray
diffraction (XRD, Rigaku) with Cu-K radiation operated at 50 KV and 300mA. The
XRD patterns were obtained with a glazing incident angle of 0.5 degree. The fieldeffect transistor device was fabricated by evaporating Au electrodes (30 nm thick)
directly on top of the selected, regularly shaped graphene sheets using a copper grid

(200 mesh, 20 m spacing) as a hardmask. The typically obtained channel length


between source and drain electrodes was around 20 m. The electrical measurements
were performed in ambient conditions using a Keithley semiconductor parameter
analyzer, model 4200-SCS.

Figure S1. The home-built annealing system with a quartz tube and a hot wall furnace.
The sample can be put on the sample hold in the quartz tube. The holder can be moved
between a hot zone (center of the furnace) and a cold zone (outside the furnace) using a
permanent as shown in the figure.

Figure S2. (a) Raman spectra for the MoS2 thin layer produced by annealing a layer of
(NH4)2MoS4 precursors on SiO2/Si substrate at 500oC as described in text. The film
obtained exhibits two characteristic MoS2 Raman peaks (E12g ~382 and A1g ~405 cm-1).
The films after first annealing were then subjected to 1000oC thermolysis in pure (Ar)
and in (Ar+S) respectively. It is observed that the Raman peak intensity is higher after
high temperature annealing. Meanwhile, the peak intensity of MoS2 further increases
with the addition of sulfur in the second annealing. (b) Photoluminescence and (c)
transfer characteristics for the MoS2 layers directly formed on SiO2/Si substrates as
mentioned above. It is observed that the MoS2 film with a higher on/off current ratio
also exhibits stronger PL and Raman peak intensity. The MoS2 film formed after 500oC
annealing (a conventional process to obtain MoS2 films) does not show any on/off
current ratio.

Figure S3. (a) Raman spectra for the micromechanically exfoliated MoS2 thin sheets
with various thickness on SiO2/Si substrates. (number of layer from 1 to 5). All spectra
were normalized by the intensity of the Si peak at 520 cm-1. (b) The Raman peak width
summarized from (a). The measurements were performed in an NT-MDT confocal
Raman system with the excitation laser 473 nm. The detailed exfoliation and
characterization for MoS2 layers is described in the reference (H. Li, et al. Small, 2012,
8, 63-67.)
.

Figure S4. (a,b) The MoS2 trilayers were respectively grown on sapphire and SiO2/Si
and then transferred on to freshly cleaned SiO2/Si substrates for spectroscopic
measurements. Both the Raman and PL intensities for the MoS2 layers grown on
sapphire are higher than those grown on SiO2/Si. (c) Typical transfer curves for the
FET devices made by two types of films. (d) Statistical measurement results showing
that the MoS2 films grown on sapphire exhibit much better electron mobility values and
on/off current ratios than those grown on SiO2/Si substrates.

Figure S5. (a,b) The selected area electron diffraction (SAED) patterns for the trilayer
MoS2 at two different locations of the film. (c) The SAED aperture size is around 160
nm in diameter. (d) The simulated SAED pattern with the lattice parameters that are
obtained from XRD: Hexagonal (P63/mmc), a=b=3.1 , C=12.8 . In the simulated
SAED patterns, the angle of between (100) and (110) is 30.

Figure S6. X-ray photoemission spectroscopy (XPS) survey scans for the MoS2
trilayers annealed with and without sulfur.

Figure S7. (a-b) AFM images for the as-grown MoS2 trilayers on sapphire and the
roughness is ~ 0.34 nm before transfer (c) AFM image of the MoS2 trilayer films after
transferred onto SiO2/Si substrates. The thickness of the film is 1.92 nm, the same as the
film before transfer. However, many wrinkles appear after the transfer process. Note
that the height of the wrinkle typically ranges from 5 to 9 nm. (d) Optical micrographs
of the MoS2 trilayer films after transferred onto SiO2/Si substrates.

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