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 Nanotechnology

Nanotechnology 32 (2021) 455705 (8pp) https://doi.org/10.1088/1361-6528/ac1756

A simple fabrication strategy for

orientationally accurate twisted
heterostructures
Rahul Debnath1,4, Shaili Sett1,4 , Rabindra Biswas3,
Varun Raghunathan3 and Arindam Ghosh1,2
1
Department of Physics, Indian Institute of Science, Bangalore 560012, India
2
Centre for Nano Science and Engineering, Indian Institute of Science, Bangalore 560012, India
3
Department of Electrical and Communication Engineering, Indian Institute of Science, Bangalore 560012,
India

E-mail: rahuldebnath@iisc.ac.in

Received 22 April 2021, revised 13 July 2021

Accepted for publication 23 July 2021
Published 18 August 2021

Abstract
Van der Waals (vdW) heterostructure is a type of metamaterial where multiple layers of 2D
materials are vertically aligned at controlled misorientation. The relative rotation in between the
adjacent layers, or the twist angle between them plays a crucial role in changing the electronic
band structure of the superlattice. The assembly of multi-layers of precisely twisted two
dimensional layered materials requires knowledge of the atomic structure at the edge of the flake.
It may be artificially created by the ‘tear and stack’ process. Otherwise, the crystallographic
orientation needs to be determined through invasive processes such as transmission electron
microscopy or scanning tunneling microscopy, and via second-harmonic generation (SHG).
Here, we demonstrate a simple and elegant transfer protocol using only an optical microscope as
a edge identifier tool through which, controlled transfer of twisted homobilayer and heterobilayer
transition metal dichalcogenides is performed with close to 100% yield. The fabricated
twisted vdW heterostructures have been characterized by SHG, Raman spectroscopy and
photoluminiscence spectroscopy, confirming the desired twist angle within ∼0.5° accuracy. The
presented method is reliable, quick and prevents the use of invasive tools which is desirable for
reproducible device functionalities.
Supplementary material for this article is available online
Keywords: Moiré superlattice, heterostructure, transition metal dichalcogenides

(Some figures may appear in colour only in the online journal)

Introduction
Van der Waals (vdW) heterostructures, where dissimilar
atomically thin vdW crystals are vertically assembled have
initiated a new paradigm to create multifunctional devices
with exciting novel physical properties [1–11]. In spite of the
weak nature of vdW interactions, unusually strong interlayer
coupling and hybridization in these heterostructures lead to
interfacial stress fields [12–14] and modification of electronic
4
These authors have contributed equally to the work.
band structure [15, 16]. In twisted van der Waals hetero-
structures (tvdWHs), the angular mismatch between two
similar lattices generates a large scale interference pattern,
known as Moiré pattern, which strongly impact the electronic
band structure of the superlattice. The Moiré pattern in
tvdWH creates a periodic potential for electrons and excitons
to yield many interesting phenomena such as Hofstadter
butterfly spectrum [17], Moiré excitons [18], tunable
Mott insulator phases [19–22], and unconventional super-
conductivity [23]. The twist angle has been shown to play a
crucial role in the optical properties of CVD grown twisted

0957-4484/21/455705+08$33.00 1 © 2021 IOP Publishing Ltd Printed in the UK

Nanotechnology 32 (2021) 455705
MoS2 [24], twisted WSe2 [25] and various heterobilayers
[18, 26, 27], and stabilizes exotic correlated phases when
maintained between 1° and 5°. At twist angles near 0°and
near 60°, ultraflat band in twisted bilayers of MoS2 has been
theoretically predicted [15, 28], and the computed bandwidths
are comparable to twisted bilayer graphene [16]. Addition-
ally, low frequency interlayer shear and breathing mode
[29–32] can emerge in twisted bilayer MoS2 (tBLM), where
periodic potential of Moiré pattern modifies the properties of
phonon of its monolayer constituent MoS2 to generate Moiré
phonons [33].
This new paradigm of vertically stacked Lego structures
with precise twist angles between the adjoining TMDC layers
requires an advanced and more generalized stacking mech-
anism. A core problem in the fabrication of these structures is
the identification of crystallographic edges of the individual
layers. The fabrication process of these tvdWH has been
mainly concentrated on the tear and stack technique and
invasive atomic force microscopy (AFM) cutting technique
which is limited to homobilayers [34]. The process of
obtaining similar atomic termination is accomplished by
using an AFM tip to cut a large flake prior to the transfer
process [35]. This process is not always feasible since it
requires a large flake of at least 20–30 μm. Also, the AFM tip
may introduce dust particles on the flake and the process of
cutting is highly dependent on the instrument parameters and
may lead to damage of the flake itself. In the case of twisted
bilayer graphene, usually the process of tear and stack
[36–38] is used to align two graphene layers. Since the edge
of an exfoliated flake can be any crystallographic orientation,
it is essential to align flakes with similar crystallographic
orientation, otherwise, the twist angle between the two layers
have an arbitrary angle, and is not the desired one. To avoid
this uncertainty, usually a hexagonal boron nitride (hBN)
flake with a sharp edge is used to partially tear a large piece of
graphene flake which is then stacked upon the remaining part.
This ensures that both the top and bottom graphene have same
atomic orientation at the edges. Only then can they be aligned
as desired. A similar process works for twisted homobilayer
TMDC, but with the restriction that it will be encapsulated by
hBN. Usually, this is an issue since edge contacts in TMDCs
are unfeasible and impractical for electronic property studies
because of high contact resistance [39]. Thus, prior identifi-
cation of the crystallographic orientation of a monolayer
TMDC flake is a necessary condition for fabrication of
tvdWH. Other techniques, like second-harmonic generation
(SHG) spectroscopy [18], scanning tunneling microscopy
[40, 41] and transmission electron microscopy [42] is
necessary for this identification. These processes are costly,
time consuming and mostly invasive in nature.
In this study, we introduce a transfer technique that
provides a better control for fabrication of homobilayers and
heterobilayers of tvdWHs. For exploring the electronic and
optical properties of tvdWH, two key aspects are necessary:
(1) layer-by-layer transfer that minimizes the incorporation of
residues at the interface which usually gather up as a ‘blister’
between layers, leading to effective decoupling between the
layers and (2) control of the crystal axes rotational alignment.
2
R Debnath et al
Our method involves quick edge identifications using an
optical microscope only and a transfer plan for aligning the
respective layers. The process relies on observation of unique
in-plane cleavage features in a TMDC flake, using which the
atomic termination at the edge of the flake can be identified
and then stacked on top of each other using dry transfer
technique. We primarily concentrate on two TMDCs, MoS2
and WSe2 as simple prototypes. Because of broken sublattice
symmetry, the Moiré pattern landscape [28] is different near
0° and 60°. Hence we demonstrate three transfer processes,
homobilayer of relative twist angle near zero degree, homo-
bilayer with relative twist angle near sixty degree and het-
erobilayer near zero degree. Post-transfer, we identify the
angle of the artificially created Moiré lattice through a com-
bination of SHG, Raman spectroscopy and PL spectroscopy
technique. Preliminary transport measurements show mobility
>300 cm2 V−1 s−1 at a bias voltage of 10 mV illustrating the
pristine quality of the devices.
Results and discussion
Edge identification
Crystalline layers of MoS2 and WSe2 were mechanically
exfoliated on 285 nm SiO2 on p++ doped Si substrate using
scotch tape technique. Single layers of MoS2 were identified
using Raman spectroscopy, invoking the difference in Raman
shift between in-plane E12g and out-of-plane A1g mode, which
is the least for a single layer (18–19 cm−1). For, WSe2, single
layers show a highly reduced second-order Raman mode due to
LA phonons (at the M point) around 260 cm−1 while a low
intensity peak at 308 cm−1 attributed to the rigid layer shear is
absent. See supporting information (SI) section 1 (available
online at stacks.iop.org/NANO/32/455705/mmedia) for ele-
mentary data for Raman spectra of monolayer flakes. Each
exfoliated flake was then observed using an optical microscope
for signatures of edge termination. MoS2 shows a high prob-
ability to cleave along zigzag direction if angles between two
straight, sharp edges are 60° or multiples of 60° [43]. This was
further confirmed from SHG measurements on the same edge.
For all SHG mapping the horizontal axis shown in white is
along the armchair direction. The zigzag orientation of the
flakes are parallel to the edges and armchair orientations are
perpendicular to the edges as shown in figure 1(a). Polarization
dependence of SHG signal is given in SI, section 1. Even in
WSe2, we observed similar behavior of zigzag edge termina-
tion. The edge termination determined by an optical image and
through SHG map in MoS2 and WSe2 are given in
figures 1(a)–(d). This in-plane cleavage behavior can be
understood by the competition between the release of elastic
energy and increase of surface energy. It is true for all other
TMDC materials. It is possible that some edge angles are not
exactly 60° but are very close to it. Since the cleavage process
is random it leads to a statistical distribution of edge angles.
For example, in figure 1(a), the edge angle is ≈60°. There are
also certain exfoliations in which the edge angles are not 60° or
its multiples. In such cases we look for other signatures such as
Nanotechnology 32 (2021) 455705 R Debnath et al

Figure 1. Crystallographic orientation of MoS2 and WSe2 monolayers determined optically from edges and verified by polarization-resolved
second-harmonic generation spectroscopy. (a) WSe2 monolayer with edge angle of 60° with orientation directions determined optically. (b)
SHG spectroscopy map of the same flake with horizontal axis showing armchair edge. The sharp edges forming 60° are zigzag. (c) MoS2
monolayer with edge angle of 60° with orientation directions determined optically. (d) SHG spectroscopy map of the same flake with
horizontal axis showing armchair edge. The sharp edges forming 60° are zigzag. (e) An MoS2 flake showing no sharp edges that form 60° but
has a clean smooth crack propagating along the flake, forming a zigzag edge. (f) SHG spectroscopy map of the same flake with horizontal
axis showing armchair edge. The crack makes 30° with the horizontal axis and is along the zigzag edge. (g) A WSe2 flake showing no sharp
edges that form 60° but has a nano scroll propagating at 90° from the bulk crystal zigzag axis, and therefore an armchair edge. (h) SHG
spectroscopy map of the same flake with horizontal axis showing armchair edge and the nano scroll making 120° with the horizontal axis.

a crack or a fold in the flake. In figure 1(e) an optical image of
a MoS2 monolayer shows a crack propagating along the flake,
making a 120° angle. The crack propagates along the zigzag
edge as has been shown in the optical image. The SHG map of
the flake in figure 1(e) has horizontal axis in the armchair
direction and the crack is 30° rotated from it, confirming zigzag
termination. It makes ≈60° with a sharp edge of the flake. In
another example, in figure 1(g) we show the optical image of a
WSe2 monolayer with no sharp edges making 60° angles.
Here, the flake shows a fold or nano scroll [44]. These features
are usually along a crystallographic direction. We observe from
the optical image, that the zigzag edge makes a 90° angle with
the direction of the nano scroll, proving that it is indeed along
the armchair direction. Another important observation is that,
the zigzag terminated edges are generally atomically smooth
while flake termination along other crystallographic directions
are disordered with dangling bonds, which in turn increase the
edge roughness. We use these parameters for quick identifi-
cation of atomic orientation in a monolayer TMDC through an
optical micrograph.
Transfer process
The transfer process involves mapping out the alignment of
the flakes to create a relative rotation between the two layers
and transferring them according to the design plan. After
identification of the zigzag edges, we proceed to plan an
alignment of the flakes with a relative twist between them.
Figures 2(a)–(e) shows overlaid micrograph of the design
plan near 0°, 60° and 180°. Since the commensurate struc-
tures near 0° and 60° are different in TMDCs, it is essential to
fabricate structures near 60°. We can also obtain a near 60°
structure by stacking it in anti-parallel configuration, which is
a 180° rotation of one flake with respect to another. This
results in AB stacking because of its three-fold crystal
symmetry.
We have used the dry transfer technique to prepare ver-
tically stacked heterostructures. We first prepare poly-
dimethylsiloxane (PDMS) stamp by mixing SYLGARD 10
parts and curing agent 1 part and putting one small droplet of
it on a clean glass cover slip. It is then baked at 150 °C for
30 min. Onto this PDMS coated glass cover slip, we spin coat
polypropylene carbonate (PPC) and cure it at 70 °C for
10 mins. The PPC is then used to pick up a flake (at 60 °C)
and capture it at 40° and then released at 100 °C onto a clean
SiO2/Si++ substrate. For aligning two layers, we use a micro-
manipulation stage, which allows rotation within an accuracy
of ≈0.1°. Figures 2(f)–(i) shows a schematic of this process.
One monolayer is first picked by PPC, and is then aligned
with a micro-manipulator stage with respect to the second
layer which is stationary. The bottom flake is then picked up.
The stack is then transferred onto a clean SiO2/Si++ sub-
strate. Figures 2(j)–(m) shows the real time optical images of
the transfer process.

3
Nanotechnology 32 (2021) 455705 R Debnath et al

Figure 2. Transfer process showing stacking of two layers of MoS2 at a desired twist angle. (a) and (b) Shows two monolayers with the
zigzag edges marked with arrows. (c)–(e) Shows the overlaid images of the two flakes with (c) near 0° twist, (d) near 60° twist and (e) near
180° twist angle between them. (f)–(i) Shows the schematic of the transfer process showing pick up of flakes and stacking them up followed
by release on SiO2/Si++ substrate. (f) 1st flake is being picked up by PPC/PDMS stamp. (g) The captured flake on the PPC layer. (h) The
second flake being picked up following the first one, after twisting. (i) The stack being transferred onto the substrate. (j)–(m) Shows the real
time optical images of the transfer process by PPC/PDMS stamp.

Avoiding of blisters during assembly SHG characterization of tvdWH

To avoid blister formation between the interfaces of the 2D
materials we tried the transfer technique at different tem-
peratures, and find that the cleanliness of the interface
depends on both the speed and temperature of the stacking
process. Stacking at 40 °C is apparently blister-free but after
heating it above 70 °C, moisture from the surrounding air is
trapped at the interface. These eventually vaporize and leads
to formation of an undulating landscape visible as blisters on
a multilayer tvdWH. The blisters are upto 50 nm tall and 2 μm
across, and evenly distributed over the sample, reducing the
interlayer coupling of the Moiré superlattice [37]. In contrast,
stacking at high temperature such as 110 °C results in a
complete absence of such blisters, but at high temperature the
folding of the flakes and lateral shift of the materials also
increase due to the reduction of viscosity of PPC, increasing
the difficulty in the sequential assembly process. Hence, we
optimized the stacking process by reducing the drop down
temperature to 60 °C and pick up temperature to 40 °C,
meanwhile limiting the speed of the contact area front to
„2 μm s−1 (video given in SI) by controlling the z-height of
the stage, resulting in a blister-free interface. AFM image of a
monolayer MoS2 flake before and after the transfer process is
given in SI, section 2 showing the ultra-clean transfer.
To validate the twist angle between the heterostructure we use
SHG measurement and find an agreement between the opti-
cally determined twist angle and that determined from SHG
microscopy within experimental error. Polarization-resolved
second-harmonic generation microscopy technique setup [45]
is used for the edge identification of monolayers and the
stacking angle measurement in artificially stacked TMDCs. In
general, monolayer TMDCs is expected to have D3h sym-
metry with nonvanishing second-order nonlinear optical
susceptibility elements given as:
c(yyy
2)
= - c(xxy
2)
= - c(yxx
2)
= - c(yyy
2)
. (1 )
Here,‘x’ and ‘y’ correspond to zigzag and armchair direction
in the crystal axis, respectively. Therefore, SHG from each
monolayer response will exhibit a six-fold symmetry for both
parallel and perpendicular polarization with SHG signal given
by [46]
I = I◦ + cos2 (3 (f + f◦)) , I^ = I◦ + sin2 (3 (f + f◦)). (2)
Here, f0 is the initial offset between the laboratory axis and
crystal y axis and f is the azimuthal angle. We have used
parallel polarization configuration for edge determination
by keeping the laser polarization, and the detector analyzer
fixed and parallel to the lab axis. the SHG images are

4
Nanotechnology 32 (2021) 455705 R Debnath et al

Figure 3. Determination of twist angle post transfer process optically and by SHG. (A) Panel shows a near zero degree twisted bilayer MoS2.
(i) and (ii) are the two monolayers used for this transfer. Their zigzag edges are verified optically by observing the angle between two sharp
edges. (iii) Shows the twisted bilayer with the zigzag axis of both flakes. The angle between the zigzag edges of the two flakes determined
from optical image is 3 ± 0.5°. (iv) SHG map showing enhancement in SHG at the overlap region, due to formation of a near zero twisted
structure. (v) Identifying the lattice direction by SHG signal on two monolayers of MoS2 (green and red circles) and the corresponding fitting
shown in curves which confirms the near zero twist angle between them. (B) Panel shows a near sixty twisted bilayer MoS2. (i) and (ii) are
the two monolayers used for this transfer. Their zigzag edges are verified optically by observing the angle between two sharp edges. (iii)
Shows the twisted bilayer transferred by anti-parallel cinfiguration. The flakes were rotated such that 180° angle forms in between the zigzag
edges. The angle between the zigzag edges of the two flakes determined from optical image is 5 ± 0.5°, corresponding to a twist angle of 55°
in between the two layers (iv) SHG map showing low intensity in SHG at the overlap region, due to formation of AB stacking. (v) Identifying
the lattice direction by SHG signal on two monolayers of WSe2 (green and red circles) and the corresponding fitting shown in curves which
confirms the near sixty twist angle between them.

obtained from the microscopy setup over an angle range of
90° degrees with respect to the lab axis by rotating the
sample placed on a rotatory mount with 5° steps. Sample
image with maximum SHG signal is then identified
corresponding to the armchair direction within an angle
error of ±0.2°.
For twist angle measurement of a tvdWH, the same
method is used where SHG image for the whole twisted
bilayer sample is obtained for different f. In case of twisted
bilayer, the net SHG emission from the stacking region will
be a coherent superposition of layers (E1µ I1 , E2µ I2 ),
along with a phase difference dependent on the stacking angle
(θ), as shown below [47]
I (q ) = I1 + I2 + 2 I1I2 cos (3q ).
Since the net SHG emission in the stacking region can be
a result of constructive or destructive interference between the
two SHG field emissions depending on the stacking angle
θ = 0° and 60°, we can easily distinguish between the AB and
AA stacking for the angle-aligned bilayer sample by com-
paring the SHG signal of the stacking region with the isolated
monolayer region. Figure 3(A) shows a tBLM transfer near
0°. The zigzag directions of both flakes are shown in
figure 3(Ai-ii). The angle between the edges, post transfer as
seen from the optical image is 3 ± 0.5°. It shows uniform,
clean transfers with no blisters in between the two TMDC
layers. The SHG map shows a higher intensity in the twisted
region, corresponding to AA type stacking. From the SHG
signal, the fit curves reveal a twist angle of 3°. For a near 60°
(3 ) transfer, we use the anti-parallel configuration technique. The

5
Nanotechnology 32 (2021) 455705 R Debnath et al

Figure 4. Characterization of twisted bilayer TMDCs using Raman and PL Spectroscopy. (a) Red shift in the E2g peak and blue shift in the
A1g peak for monolayer MoS2 and twisted bilayers at various angles. (b) Room temperature PL Spectroscopy of MoS2 twisted layers
showing presence of indirect excition peak I, which is absent in monolayer. The 60° twisted sample refers to a natural bilayer which has
indirect exciton peak at 1.5 eV. (c) Low temperature PL Spectroscopy of WSe2. The natural bilayer (60° shows indirect exciton peak XI) at
1.56 eV which is highly reduced for the homobilayer twisted at 20° and completely absent for the monolayer. The other peaks between 1.7
and 1.8 eV are intralayer excitions (X0).

zigzag edges are aligned at 180° to each other as shown in
figure 3(B). The twist angle between the two edges post
transfer is determined optically to be 5°. This corresponds to a
twist of 60–5 = 55° in real space. The fit to SHG signal shows
a 5° twist angle between the layers. Other transfer plans and
results using WSe2, MoS2, WS2 and heterobilayers are given
in SI (section 3). SHG on the twisted bilayer heterostructures
reveals the exact angle between the two layers within an
accuracy of 0.2° which matches well with the optically
determined twist angle within an accuracy of 0.5°. The twist
angle is measured during the transfer process through the
rotational stage, post-transfer from the optical image as well
as after overlapping the image of the monolayers on the
optical image of the heterostructure. Multiple measurements
introduce a total error of ±0.5° to the twist angle from the
optical micrograph.
Twisted bilayer characterizations
The twisted homobilayer TMDCs, MoS2 and WSe2 has been
characterized by Raman, PL and SHG. We show that SHG is
not necessary to ascertain the twist angle between two layers.
It can be adjudged from the optical micrograph image of the
twisted flakes and from Raman and PL spectroscopy. Inter-
action between two layers not only modifies the electronic
band structure but also the phonon vibrations in them. Raman
studies on MoS2 shows that the separation between the two
peaks (E2g and A1g) can effectively characterize the interlayer
mechanical coupling between layers [45]. Larger separation
[48] (25 cm−1, seen in bulk MoS2) corresponds to greater
coupling between layers. Figure 4(a) shows the Raman peak
separation in twisted bilyaer MoS2 which has a larger
separation compared to monolayer by almost 3–4 cm−1 and is
similar or greater than bilayer MoS2. PL spectrum (shown in
figure 4(b)) of a monolayer MoS2 [24, 49, 50] shows a high
intensity peak at ∼1.85 eV and a lower intensity peak at
∼2.05 eV, which may be fitted by three Lorentzians
corresponding to A exciton, A− trion and B exciton (fits to the
PL data are given in SI, section). It corresponds to the well
known excitonic transition at the K-valley of the Brillouin
zone [51]. For a bilayer TMDC, in addition to this, we
observe a lower intensity peak around 1.5 eV corresponding
to a momentum indirect interlayer exciton [24, 52] (XI) peak
which reflects the electronic coupling strength and leads to
hybridization of the electronic band in the Brilloiun zone. The
tBLM transfers near 0° and 60° show the XI peak between
1.45 and 1.55 eV. The presence of this peak is a clear indi-
cation that the twisted layers have strong coupling between
them [52]. Figure 4(c) shows similar PL spectra of the
monolayer WSe2 as well as twisted WSe2 at 7 K temperature,
showing prominent indirect exciton [53–55] which indicates
strong interlayer hybridization due to Moiré potential.
Electrical characterization
The quality of transfer in the tvdWH were confirmed through
electrical measurements in field-effect transistor (FET) con-
figuration. Figure 5(a) shows the optical micrograph of tBLM
at an angle of 55°. Figure 5(d) shows linear output char-
acteristics between electrodes 1 and 3 as shown in figure 5(b)

6
Nanotechnology 32 (2021) 455705
Figure 5. Electrical characterization of 55° twisted bilayer MoS2 at room temperature. (a) Optical image of the twisted bilayer MoS2.
(b) Optical image after fabrication of Cr/Au electrodes. (c) Schematic of the device structure. (d) Ids versus Vds curves for different back gate
voltages. (e) Transfer characteristics for Vds = 10 mV. (f) Field effect mobility of the twisted MoS2 device as a function of gate voltage.
of the twisted bilayer FET at different gate voltages, showing
the absence of Schottky barrier at room temperature. In
figure 5(e) We show the variation of source-drain current (Ids)
as a function of backgate voltage (Vbg) with forward and
backward sweep. It shows negligible hysteresis, implying
minimal potential fluctuations. The conductance was achieved
at the positive gate voltage implying n-type transport
behavior. Field effect mobility is also extracted from the
transfer characteristics, showing values >300 cm2 V−1 s−1
(figure 5(f)) at 10 mV source-drain bias (Vds), implying less
scattering due to impurity [56–58]. This demonstrates the
quality of devices which is essential for low temperature
electronic transport measurements.
Conclusion
In summary, we have presented a simple, controllable method
for rapid fabrication of tvdWH, with a twist angle measure-
ment accuracy of 0.5° which can be determined solely by
optical microscopy. This generalized method can pave the
way for fabrication of high quality, controllable twisted
tvdWH without use of expensive and elaborate edge identi-
fication tools. For accurate crystallographic edge identifica-
tion, observing the optical micrograph for unique features is
sufficient. We have illustrated the validity of the technique by
performing SHG spectrosocpy on these tvdWHs and it is in
quantitaive agreement with what is determined optically. The
tvdWH show high mobility at room temperature which
authenticates a clean transfer process. Our comprehensive
7
R Debnath et al
rapid and ultra-clean transfer process will be beneficial to
fabricate twisted TMDCs where correlated physics is still
largely unexplored.
Materials and methods
Experiment
PL and Raman spectroscopy: Raman and PL spectra of
MoS2 flakes were done by using Horiba LabRAM HR
spectrometer. 532 nm laser with laser power less than 1.5 mW
was used for spectroscopy measurement.
SHG measurements: A femtosecond laser (Fidelity HP-
10 laser, 80 MHz repetition rate, wavelength at 1040 nm and
pulse duration of 140 fs) was used as the light source. We
used 4 mW linearly polarized light focused to a diameter of
1 μm for excitation, and collected the SHG signal using a
spectrometer coupled with a charge-coupled device.
Acknowledgments
The authors thank the financial support from the Department
of Science and Technology, Government of India and
Supercomputer Education and Research Center (SERC) at
IISc for providing computational resources. The authors also
thank the Ministry of Electronics and Information Technol-
ogy, Government of India. The authors acknowledge financial
support from U.S. Army International Technology Center
Pacific (ITC-PAC).
Nanotechnology 32 (2021) 455705
Data availability statement
All data that support the findings of this study are included
within the article (and any supplementary files).
Notes
The authors declare no competing financial interests.
ORCID iDs
Shaili Sett https://orcid.org/0000-0001-6739-8090
Varun Raghunathan https://orcid.org/0000-0002-
0141-4032
References
[1] Wang Q H, Kalantar-Zadeh K, Kis A, Coleman J N and
Strano M S 2012 Nat. Nanotechnol. 7 699
[2] Cui X et al 2015 Nat. Nanotechnol. 10 534
[3] Rosenberger M R, Chuang H-J, Phillips M, Oleshko V P,
McCreary K M, Sivaram S V, Hellberg C S and Jonker B T
2020 ACS Nano 14 4550
[4] Roy K, Padmanabhan M, Goswami S, Sai T P, Ramalingam G,
Raghavan S and Ghosh A 2013 Nat. Nanotechnol. 8 826
[5] Jadczak J, Bryja L, Kutrowska-Girzycka J, Kapuściński P,
Bieniek M, Huang Y-S and Hawrylak P 2019 Nat. Commun.
10 1
[6] Mahapatra P S, Ghawri B, Garg M, Mandal S, Watanabe K,
Taniguchi T, Jain M, Mukerjee S and Ghosh A 2020 Phys.
Rev. Lett. 125 226802
[7] Mahapatra P S, Sarkar K, Krishnamurthy H, Mukerjee S and
Ghosh A 2017 Nano Lett. 17 6822
[8] Chakraborty B, Gu J, Sun Z, Khatoniar M, Bushati R,
Boehmke A L, Koots R and Menon V M 2018 Nano Lett.
18 6455
[9] Ahmed T, Bellare P, Debnath R, Roy A, Ravishankar N and
Ghosh A 2020 ACS Nano 14 5909
[10] Paul T, Ahmed T, Tiwari K K, Thakur C S and Ghosh A 2019
2D Mater. 6 045008
[11] Jayaraman A, Hsieh K, Ghawri B, Mahapatra P S,
Watanabe K, Taniguchi T and Ghosh A 2021 Evidence of
lifshitz transition in the thermoelectric power of ultrahigh-
mobility bilayer graphene Nano Lett. 21 1221–7
[12] Zhu S and Johnson H T 2018 Nanoscale 10 20689
[13] Lin X, Liu D and Tománek D 2018a Phys. Rev. B 98 195432
[14] Ahmed T, Naik M H, Kumari S, Suman S P, Debnath R,
Dutta S, Waghmare U V, Jain M and Ghosh A 2019 2D
Mater. 6 041002
[15] Naik M H and Jain M 2018 Phys. Rev. Lett. 121 266401
[16] Tarnopolsky G, Kruchkov A J and Vishwanath A 2019 Phys.
Rev. Lett. 122 106405
[17] Hunt B et al 2013 Science 340 1427
[18] Jin C et al 2019 Nature 567 76–80
[19] Po H C, Zou L, Vishwanath A and Senthil T 2018 Phys. Rev. X
8 031089
[20] Bistritzer R and MacDonald A H 2011 Proc. Natl Acad. Sci.
108 12233
[21] Cao Y et al 2018a Nature 556 80
[22] Wang L et al 2020 Nat. Mater. 19 861–6
R Debnath et al
[23] Cao Y, Fatemi V, Fang S, Watanabe K, Taniguchi T,
Kaxiras E and Jarillo-Herrero P 2018b Nature 556 43
[24] Liu K, Zhang L, Cao T, Jin C, Qiu D, Zhou Q, Zettl A, Yang P,
Louie S G and Wang F 2014 Nat. Commun. 5 4966
[25] Andersen T I et al 2019 Excitons in a reconstructed moiré
potential in twisted WSe2/WSe2 homobilayers Nat. Mater.
20 480–7
[26] Tran K et al 2019 Nature 567 71
[27] Alexeev E M et al 2019 Nature 567 81
[28] Naik M H, Kundu S, Maity I and Jain M 2020 Phys. Rev. B
102 075413
[29] Huang S, Liang L, Ling X, Puretzky A A, Geohegan D B,
Sumpter B G, Kong J, Meunier V and Dresselhaus M S
2016 Nano Lett. 16 1435
[30] Puretzky A A, Liang L, Li X, Xiao K, Sumpter B G,
Meunier V and Geohegan D B 2016 ACS Nano 10 2736
[31] Zhao Y et al 2013 Nano Lett. 13 1007
[32] Liang L, Zhang J, Sumpter B G, Tan Q-H, Tan P-H and
Meunier V 2017 ACS Nano 11 11777
[33] Lin M-L et al 2018b ACS Nano 12 8770
[34] Saito Y, Ge J, Watanabe K, Taniguchi T and Young A F 2020
Nat. Phys. 16 926
[35] Chen G et al 2019 Nat. Phys. 15 237
[36] Kim K et al 2016 Nano Lett. 16 1989
[37] Pizzocchero F, Gammelgaard L, Jessen B S, Caridad J M,
Wang L, Hone J, Bøggild P and Booth T J 2016 Nat.
Commun. 7 1
[38] Cao Y, Luo J, Fatemi V, Fang S, Sanchez-Yamagishi J,
Watanabe K, Taniguchi T, Kaxiras E and Jarillo-Herrero P
2016 Phys. Rev. Lett. 117 116804
[39] Jain A, Szabó Á, Parzefall M, Bonvin E, Taniguchi T,
Watanabe K, Bharadwaj P, Luisier M and Novotny L 2019
Nano Lett. 19 6914
[40] Pan Y, Folsch S, Nie Y, Waters D, Lin Y-C, Jariwala B,
Zhang K, Cho K, Robinson J A and Feenstra R M 2018
Nano Lett. 18 1849
[41] Zhang C, Chen Y, Johnson A, Li M-Y, Li L-J, Mende P C,
Feenstra R M and Shih C-K 2015 Nano Lett. 15 6494
[42] Yuan L, Zheng B, Kunstmann J, Brumme T, Kuc A B, Ma C,
Deng S, Blach D, Pan A and Huang L 2020 Nat. Mater.
19 617
[43] Guo Y et al 2016 ACS Nano 10 8980
[44] Qian Q, Zu R, Ji Q, Jung G S, Zhang K, Zhang Y, Buehler M J,
Kong J, Gopalan V and Huang S 2020 ACS Nano 14 13333
[45] Debnath R, Maity I, Biswas R, Raghunathan V, Jain M and
Ghosh A 2020 Nanoscale 12 17272
[46] Li Y, Rao Y, Mak K F, You Y, Wang S, Dean C R and
Heinz T F 2013 Nano Lett. 13 3329
[47] Hsu W-T, Zhao Z-A, Li L-J, Chen C-H, Chiu M-H, Chang P-S,
Chou Y-C and Chang W-H 2014 ACS Nano 8 2951
[48] Lee C, Yan H, Brus L E, Heinz T F, Hone J and Ryu S 2010
ACS Nano 4 2695
[49] Huang S, Ling X, Liang L, Kong J, Terrones H, Meunier V and
Dresselhaus M S 2014 Nano Lett. 14 5500
[50] Zhang X, Zhang R, Zhang Y, Jiang T, Deng C, Zhang X and
Qin S 2019 Opt. Mater. 94 213
[51] Mak K F, He K, Lee C, Lee G H, Hone J, Heinz T F and Shan J
2013 Nat. Mater. 12 207
[52] van Der Zande A M et al 2014 Nano Lett. 14 3869
[53] You Y, Zhang X-X, Berkelbach T C, Hybertsen M S,
Reichman D R and Heinz T F 2015 Nat. Phys. 11 477
[54] Merkl P et al 2020 Nat. Commun. 11 1
[55] Scuri G et al 2020 Phys. Rev. Lett. 124 217403
[56] Ghatak S, Pal A N and Ghosh A 2011 ACS Nano 5 7707
[57] Radisavljevic B and Kis A 2013 Nat. Mater. 12 815
[58] Liu W, Sarkar D, Kang J, Cao W and Banerjee K 2015 Acs
Nano 9 7904