Journal of ELECTRONIC MATERIALS, Vol. 46, No.

7, 2017
DOI: 10.1007/s11664-016-5037-9
Ó 2016 The Minerals, Metals & Materials Society

Coincidence Lattices and Interlayer Twist in van der Waals

Heterostructures: Application of the Coincidence Lattice Method
on hBN/MoSe2 Heterobilayer Systems

DANIEL S. KODA1,3 FRIEDHELM BECHSTEDT,2,5

MARCELO MARQUES,1,4 and LARA K. TELES1,4

1.—Group of Semiconductor Materials and Nanotechnology, Instituto Tecnológico de Aeronáutica,

DCTA, 12228-900 São José dos Campos, Brazil. 2.— Institut für Festkörpertheorie und
-optik, Friedrich-Schiller-Universität, Max-Wien-Platz 1, 07743 Jena, Germany. 3.—e-mail:
danielskoda@gmail.com. 4.—e-mail: gmsn@ita.br. 5.—e-mail: friedhelm.bechstedt@uni-jena.de

Van der Waals heterostructures have great potential in large-scale integration

devices and exploration of new physics. Experimental investigations allow
flexible combinations of two-dimensional crystals in device fabrications. The-
ory, however, has limitations of supercell sizes and commensurability,
translated into computational effort. In this work, we demonstrate the
application of the coincidence lattice method to simulate two hBN/MoSe2
heterobilayers taking interlayer twist effects into account. We predict that
both systems are stable upon contact and interact via van der Waals disper-
sions. We found that electronic properties of MoSe2 are preserved for both
simulated systems, but hBN suffers from the increase of interface interac-
tions, as evidenced by band structures and density of states calculations. Fi-
nally, band discontinuities are obtained and charge transfer arguments
explain small shifts in band offsets with respect to natural alignments. We
conclude that hBN is a reasonable substrate for preserving useful properties of
MoSe2 for application in electronic and optoelectronic devices, and that
interlayer twist angles play a significant role in the physics of van der Waals
heterostructures.

Key words: hBN, MoSe2 , coincidence lattice method, interlayer twist,

vdW heterostructures

INTRODUCTION devices,6 quantum wells7 and band alignment

engineering.8
The study of new two-dimensional (2D) materials
Another group of widely studied and interesting
over the last decade has expanded horizons for new
materials are transition metal dichalcogenides
electronics and its applications in spintronics, opto-
(TMDCs). Their unique electronic properties
electronics, solar cells, batteries and so on.1 Among
include layer-dependent band gap in the visible
the most popular 2D crystals is hexagonal boron
spectrum, which allows band engineering for flexi-
nitride (hBN). Its insulating properties in a mono-
ble and transparent optoelectronic devices and field-
layer crystal are used for enhanced dielectrics,2
effect transistors (FET).9,10 Molybdenum dichalco-
interface decoupling,3 avoidance of chemical degra-
genides are well-known examples of useful semi-
dation4 and tunneling barriers.5 The huge band gap
conducting compounds for electronic devices. FET
is also promising for ultraviolet optoelectronic
fabricated with MoS2 have displayed a current on/
off ratio as high as 108 and low power consump-
tion,11 while photosensitive devices have shown
(Received July 15, 2016; accepted October 6, 2016;
improved response when compared with gra-
published online November 3, 2016) phene.12 Molybdenum diselenide (MoSe2 ), on the

3910
Coincidence Lattices and Interlayer Twist in van der Waals Heterostructures: Application
of the Coincidence Lattice Method on hBN/MoSe2 Heterobilayer Systems
other hand, exhibits a direct optical band gap of
1.55 eV, which is close to the optimal value for solar
cell applications.13 Moreover, FET manufactured
with MoSe2 have also been reported, displaying
properties such as high temperature dependence14
and low noise.15
Different semiconductors can be assembled to
take advantage of the amalgamated properties. In
the case of 2D materials, one efficient way of doing
this is by stacking the layers to form van der Waals
(vdW) heterostructures.16 The wide library of 2D
crystals and the absence of lattice-matching con-
straints on vdW stacks broaden the possibilities for
novel devices based on interface modulation, such as
hBN-based quantum wells.17,18 Experimental tech-
niques such as mechanical exfoliation of layered
crystals favor preparation of vdW heterostructures
for different combinations of materials and orienta-
tions. Effects such as interlayer twist and incom-
mensurability may induce changes in the structural
and electronic properties of the system.19,20
Theory can help in understanding novel
heterostructures. Numerical simulations of vdW
heterostructures are only possible in commensu-
rable systems. In most cases, forcing a commensu-
rability implies dealing with long-range
periodicities in real space by using Bravais super-
lattices or some strain. In the first case, the size of
the supercell greatly increases the computational
efforts necessary to analyze the system within the
density functional theory (DFT).21 On the other
hand, the application of an artificial strain may
incorrectly describe the electronic properties of the
materials when simulating vdW heterostruc-
tures.22,23 These trade-offs are optimized by employ-
ing the coincidence lattice method,24 which
demonstrates its effectiveness by obtaining smaller
supercells within twisted systems.
In this work, we analyze structural and electronic
properties of two hBN/MoSe2 twisted bilayer sys-
tems predicted using the coincidence lattice method.
By means of ab initio calculations within the DFT,
we show that both systems form a weakly-interact-
ing heterojunction via vdW bonds. Band structures
and density of states indicate that the direct band
gap of MoSe2 is preserved upon contact with hBN
for both simulated angles. Electronic properties of
hBN such as its band gap, however, are influenced
by the rotation. Finally, band discontinuities are
calculated and shifts in natural band offsets are
explained by means of charge transfer.
METHODOLOGY
DFT calculations are performed using the Vienna
Ab-initio Simulation Package25,26 implemented with
the projector-augmented wave (PAW) method.27,28
The Perdew–Burke–Ernzerhof (PBE) functional29 is
employed to describe exchange and correlation
potential. All structural relaxations take van der
Waals interaction into account by using the optB86b
3911
functional.30 Integrations over the Brillouin zone
use a 12  12  1 C-centered Monkhorst-Pack k-
points mesh31 even for supercells. Density of states
calculations use a 32  32  1 k-points mesh and are
modeled using the tetrahedron method with Blöchl
corrections.32 The kinetic energy cutoff is fixed to
500 eV and all 2D systems are calculated with a
vacuum of thickness larger than 20 Å. The energy
convergence criterion is 105 eV and atomic posi-
tions of all systems are relaxed until Hellmann-
Feynman forces on atoms are smaller than 1 meV/Å.
Visualizations of supercells and structures are made
with the software VESTA.33
The coincidence lattice method24 consists in a
powerful tool to predict favorable supercells by
solving a system of linear diophantine equations.
Starting from a set fa1 ; a2 ; c1 ; c2 g of lattice vectors
from known 2D crystals, it is possible to find
coincidences which require little strain if a rotation
is allowed. Thus, given a rotation matrix M and two
crystals, solving Eq. 1 as in Ref. 24,
   
m1 n1
½ a1 a2  ¼ M ½ c1 c2  ; ð1Þ
m2 n2
for the integers ðm1 ; m2 ; n1 ; n2 Þ within a range of
tolerance and size, it is possible to minimize super-
cell sizes and computational efforts when simulat-
ing systems derived from these coincidences. Details
of the method are given in Ref. 24, in which more
than 700 feasible heterostructures are demon-
strated with less than 100 atoms/supercells and
strain inferior to 1%.
RESULTS AND DISCUSSION
We start from the DFT-optimized 2D crystals and
their Bravais lattices. According to predictions in
Ref. 24, if a hBN/MoSe2 heterobilayer would be
constructed without taking rotations into account, a
(4  4) hBN and (3  3) MoSe2 supercell could be
built if both layers were subjected to a biaxial strain
of 0.73%, compressive for hBN and tensile for
MoSe2 . Furthermore, a supercell with 59 atoms
would
pffiffiffi have
pffiffiffi to be simulated.

Creating a supercell of
a ( 7  7ÞR19.1 hBN on (2  2) MoSe2 , however,
reduces the strain to make the system commensu-
rate to an absolute value of 0.33% on both layers,
still compressive for hBN and tensile for MoSe2 .
This supercell contains 26 atoms inside itself and is
depicted in Fig. 1a. To further p expand
ffiffiffiffiffiffi pinvestiga-
ffiffiffiffiffiffi
tions concerning
pffiffiffi pffiffiffi rotations, a ( 12  12ÞR30.0
hBN on ( 7  7ÞR19.1 MoSe2 supercell can be
created to minimize the strain necessary to make
the system almost commensurate, as a biaxial
strain as small as 0.18% on both layers would be
enough to create the supercell. This last system is
still smaller than the aligned heterobilayer super-
cell, with 45 atoms to be taken in consideration, and
is represented by Fig. 1b. In this work, we simulate
the last two systems, designated by their relative
3912
interlayer twist angle of 19:1 and 10:9 , due to their
lower strain and size compared to the aligned
system. In order to preserve the electronic proper-
ties of the strain-sensitive MoSe2 ,34 such as its
direct band gap, we apply all the strain on hBN.
This leads to biaxial strains on this layer of 0:67%
(0.37%) for the 19:1 (10:9 ) rotated system. The
applied strain has small influences on the electronic
properties of hBN. This commensurability strain
shifts the conduction band minimum (CBM)
upwards (downwards) by 0.05 eV (0.04 eV) and the
valence band maximum (VBM) downwards (up-
wards) by 0.02 eV (0.01 eV) for the 0:67%
(0.37%) strain case. The tensile strain of 0.37% on
hBN also leads to a indirect to direct band gap
transition.
The stability for both bilayer systems is investi-
gated first by varying the interlayer distance and
obtaining the energy as a function of the separation
while keeping the atoms fixed in their positions
within the monolayers. These curves for the
Fig. 1. Coincidence lattices and atomic representation for the
MoSe2 /hBN heterobilayer for interlayer twist angles of (a) 19:1 and
(b) 10:9 .Blue (green) hexagons with solid (dashed) lines depict
MoSe2 (hBN) Bravais lattices, respectively, while dark blue, light
blue, light green and dark green circles depict molybdenum, sele-
nium, boron and nitrogen atoms, respectively. Coincidence lattices
are highlighted with green hexagons as a guide to the eye.
Koda, Bechstedt, Marques, and Teles
simulated structures are shown in Fig. 2. The
binding energy Eb is given by
ðEMoSe2 þ EhBN Þ  Ehet
Eb ¼ ; ð2Þ
Asupercell
in which Ehet is the total energy of the heterobilayer
for a given interlayer distance, EMoSe2 and EhBN are
the energies of the strained and isolated MoSe2 and
hBN monolayers considering their positions to form
the heterostructure, and Asupercell is the area of the
supercell. Therefore, no contribution due to the
elastic energy is included in the binding energy, and
the binding energy curve only takes into account the
contact energy to analyze effects of rotation into the
weak vdW binding. For each of the two interlayer
twist angles investigated, a minimum is found.
Then, letting the heterobilayers with an interlayer
distance that minimizes the energy of the systems,
i.e. their most stable configuration, atomic positions
are relaxed. Both systems are almost identical when
considering their binding energy curves, with a
binding energy of 21.2 meV/ Å 2 (21.1 meV/Å 2 ) for a
relative rotation angle of 19:1 (10:9 ). These values
are reasonable for molybdenum diselenides.35 Inter-
layer twists do not induce significant changes in the
equilibrium distance of the bilayer system because
of the planar structure of hBN, for which no
preferential stacking is found within the heterobi-
layer. Nevertheless, vdW interactions assure the
stability with the same binding energy regardless of
the interlayer twist angle.
For both heterobilayers on their respective equi-
librium positions, band structures are projected
onto atomic sites and represented with colors to
allow better interpretations of band formations, as
depicted in Fig. 3. Projected bands from each
monolayer differ from the ones of their 1  1 cells
Fig. 2. Binding energy curves for the MoSe2 /hBN heterobilayer
system for interlayer twist angles of 19:1 (solid black line) and 10:9
(dashed red line). The equilibrium distance for the 19:1 (10:9 ) ro-
tated system is 3.44 Å(3.48 Å) and the binding energy for the most
stable configuration is 20.9 meV/Å2 (21.1 meV/Å2 ) if no relaxation in
atomic positions is performed.
Coincidence Lattices and Interlayer Twist in van der Waals Heterostructures: Application 3913
of the Coincidence Lattice Method on hBN/MoSe2 Heterobilayer Systems

due to band foldings that occur onto the first " #  

Brillouin zone (1BZ) when using a supercell to k~1 k1
calculate band structures. In order to understand ¼ B1 M T B : ð11Þ
k~2 k2
band foldings in arbitrary monolayer supercells, let
k be a point in the 1BZ, written as a linear
combination of a reciprocal lattice vector basis When the methodology from Eqs. 3 to 11 is
ðb1 ; b2 Þ as employed to calculate the symmetry points for the
supercells, it becomes clear that both the K and M
k ¼ k1 b1 þ k2 b2 : ð3Þ points ofpthe ffiffiffiffiffi
ffiffiffiffiffiffi 1p 1ffi hexagonal BZ are folded onto C
for a ð 12  12ÞR30 hexagonal supercell. An
We start from the three-dimensional vector basis immediate consequence
pffiffiffiffiffiffi pffiffiffiffiffiisffi that the direct band gap
ða1 ; a2 ; a3 Þ and use the definition of reciprocal lattice of monolayer ð 12  12ÞR30 hBN on K is folded
vectors from Ashcroft and Mermin,36 onto C. Other relevant symmetry foldings for super-
( a2 a3 cells used in this work are described in Table I.
b1 ¼ 2p a1 ða 2 a3 Þ Therefore, the use of monolayer supercells neces-
a3 a1 : ð4Þ
b2 ¼ 2p a1 ða sary for the construction of heterostructure cells
2 a3 Þ
may change the presentation of band structures
when compared with the original ones due to
The 2D Bravais lattice requires only two vectors folding. Analysis of electronic properties must be
to be described. Therefore, a3 may be adopted as done having in mind that original monolayer super-
½0 0 1T and the definitions from Eq. 4 reduced to two cells lead to different foldings when band structures
dimensions by simplifying the cross product. This are plotted, and that this procedure does not
leads to interfere with electronic properties of each material.
8   On the other hand, since coincidences between two
>
> 2p
a2y Bravais lattices define unit cells for heterostruc-
> b1 ¼ det A
>
< a2x tures, band structures for the interface such as the
 ; ð5Þ ones depicted in Fig. 3 should not be interpreted as
>
> a1y
>
> b2 ¼ 2p folded. Rather, no redundancy is presented within
: det A these band structures and no further simplifications
a1x
in which are allowed.
  For both simulated systems, the direct band gap
a1x a2x of MoSe2 is retained and does not deviate from the
A ¼ ½ a1 a2  ¼ : ð6Þ value of 1.50 eV obtained by simulation of the
a1y a2y
isolated monolayer. This illustrates an important
advantage for the use of hBN as a substrate for
Finally, the reciprocal lattice vectors can be optoelectronic applications using this TMDC. On
written as the other hand, electronic properties of hBN differ
  when rotation is included. An analysis of the
2p a2y  a1y
B ¼ ½ b1 b2  ¼ ¼ 2pAT : ð7Þ heterostructure bands by means of orbital composi-
det A a2x a1x tion indicates an out-of-plane overlapping of pz
orbitals from the hBN layer with dxz and dyz orbitals
Suppose the Bravais lattice symmetry is pre- from MoSe2 layer. Interlayer interactions, there-
served with a linear transformation, i.e. an opera- fore, may decrease the band gap projected onto hBN
tion M is applied to both direct lattice vectors a1 , a2 . due to the formation of hybrid bands with contribu-
The new lattice vectors are, therefore, described by tions of both monolayers. However, an interlayer
twist of 19:1 keeps sharper distinctions between
A~ ¼ MA ¼ ½ a~1 a~2  ¼ ½ Ma1 Ma2 ; ð8Þ hBN and MoSe2 conduction bands in the k-space, as
can be seen in the projected bands of Fig. 3a. This
and the reciprocal lattice is transformed into
can be compared to the mixed-contributions con-
B~ ¼ 2pðMAÞT ¼ 2pM T AT : ð9Þ duction bands at C in the k-space when an angle of
10:9 is imposed to the heterobilayer to assume that
relative rotations can influence electronic properties
Therefore, the coordinates of the point k after the of the monolayer hBN substrate. The opposite effect
change of basis, denoted here by k, ~ seems to happen to the valence band. The 19:1 -
" # rotated bilayer presents more interlayer overlap,
~
~ ¼ k~1 b~1 þ k~2 b~2 ¼ B~ k1 ;
k ð10Þ
which is seen in Fig. 3a next to the K point for
k~2 energies close to 5:8 eV. Meanwhile, the hBN
valence band for the 10:9 system distinguishes
are calculated by itself from the MoSe2 bands.
3914 Koda, Bechstedt, Marques, and Teles

Table I. Folding symmetry for 1BZ points in hexagonal supercells

Supercell Original point Folded onto point

11 K K
M M
22 K K
pffiffiffi pffiffiffi M C
( 7  7ÞR19.1 K K
pffiffiffiffiffiffi pffiffiffiffiffiffi M M
( 12  12ÞR30 K C
M C
Original point corresponds to the symmetry point as seen in a 1  1 cell. When the linear operation described in the Supercell column is
applied to the unit system, the original point is folded onto the 1BZ according to the relationship shown in the Folded onto point column.

(a) (b)

Fig. 3. Projected band structures for the MoSe2 /hBN heterobilayer system with an interlayer twist angle of (a) 19:1 and (b) 10:9 . Blue triangles
and green circles depict contributions from MoSe2 and hBN, respectively, to the specific eigenvalue for each k-point. Greater relative contri-
butions are represented by larger markers. The vacuum level of the MoSe2 side is set as the reference and the red line identifies the top of the
valence band.

The analysis of the density of states (DOS) for

both systems agrees with this inferences. Figure 4
shows the density of states calculated for both (a)
bilayer heterostructures, from which three impor-
tant features can be noted. Firstly, the MoSe2 DOS
is not influenced close to the valence and conduction
bands for both heterobilayers, thus underpinning
the preservation of electronic properties of this
TMDC upon contact with hBN. Secondly, the con-
duction band of hBN can be distinguished from the
overlapped states with MoSe2 bands because of the
falling edge followed by a rising edge at 1:25 eV. (b)
Evidently, the DOS for hBN above the CBM should
be substantially greater than zero. The same cannot
be seen in the 10:9 rotated system, which has a
non-zero density of states for energies above
1:50 eV. Furthermore, the magnitude of the DOS
for energies close to the CBM of hBN is close to that
from hBN itself, indicating the presence of signifi-
cant hBN states above 1:50 eV. Finally, the den-
sity of states for the valence band of both systems
Fig. 4. Density of states for the MoSe2 /hBN heterostructure with an
show that a step-like DOS for the VBM of hBN in interlayer twist of (a) 19:1 and (b) 10:9 . Gray, blue and green lines
the 10:9 system is coherent with the low-interfer- depict total states, states from the MoSe2 and from the hBN layers.
ence between bands. Alternatively, the valence The vacuum level of the MoSe2 side is set as the reference.
band analysis for the 19:1 heterobilayer shows
Coincidence Lattices and Interlayer Twist in van der Waals Heterostructures: Application
of the Coincidence Lattice Method on hBN/MoSe2 Heterobilayer Systems
that the spiky DOS should be consequence of
interlayer effects for bands close to this energy.
With the electrostatic potential of the vacuum set
as the reference for all calculations, it is possible to
make a comparison between the band discontinu-
ities given by the separated layers (the natural band
alignment) and the band offset of the calculated
heterostructure. However, charge transfer effects
must be taken into consideration by means of the
dipole step in the vacuum level. In both simulated
heterobilayers, the vacuum on the MoSe2 side is
taken as reference. With respect to this zero, CBM
and VBM of MoSe2 do not shift when compared to
its natural alignments. However, hBN suffers a
shift down, as the VBM shifts downwards by
0.25 eV (0.44 eV) with respect to their VBM for
their 0:66% (0.37%) strained and isolated counter-
parts simulated within the 19:1 (10:9 ) systems.
This shift could also be responsible for enhancing
interlayer interactions in both heterobilayers,
specifically for the conduction band, and partly
due to the charge transfer between the two layers.
We report a ratio between the conduction and
valence band of approximately 80:20 (75:25) for
the 19:1 (10:9 ) system. Figure 5a and b summa-
rizes this findings. These effects on band disconti-
nuities can be explained by means of charge
transfer mechanisms. By using the differential
charge density given by
ZZ
DqðzÞ ¼ qhet ðx; y; zÞ dx dy
ZZ ZZ
qMoSe2 ðx; y; zÞ dx dy  qhBN ðx; y; zÞ dx dy;
ð12Þ
and the total charge transferred as a function of the
z position,
Z z
QðzÞ ¼ DqðnÞ dn; ð13Þ
0 upon contact with hBN, demonstrating great poten-
a charge transfer analysis can be plotted as in
Fig. 5c. For both analogous systems, electrons are
transferred from the hBN layer to the MoSe2 layer,
creating a dipole in the interface. Evaluating Q(z) in
the interface between hBN and MoSe2 , it can be
seen that the charge is negative. This means hBN is
depleted from electrons, while MoSe2 receives elec-
trons. Thus, the positive electric charge in hBN
shifts down the band edges, in agreement with the
dipole step in the interface.
CONCLUSION
In summary, we demonstrate the application of a
useful methodology for theoretical investigation of
vdW heterostructures concerning interlayer twist
and supercells requiring low computational efforts.
The coincidence lattice method is employed to
simulate MoSe2 /hBN heterobilayers with small
supercells and taking interlayer twists of 19:1
3915
(a) (b)
(c)
Δρ
Fig. 5. Band alignments (in eV) calculated with respect to the vac-
uum level for the hBN/MoSe2 bilayer when an interlayer twist angle
of (a) 19:1 and (b) 10:9 is taken into account. The natural band
discontinuities for hBN are from the 0:67% (0.37%) strained
monolayers which form the 19:1 (10:9 ) heterobilayer. (c) Differ-
ential charge density (Dq, black solid lines) and transferred charge
(Q, red dashed lines) for the 19:1 bilayer system. Positions of the
hBN and MoSe2 layers are represented with the individual cells. The
10:9 system is analogous and is suppressed.
and 10:9 into account. Small strains were applied
to the hBN layer to make the system commensu-
rate, slightly modifying natural band discontinu-
ities. Both systems have almost equal binding
energy and are stabilized by weak vdW interactions.
Electronic properties are simulated for both rotated
systems. The direct band gap of MoSe2 is preserved
tial for optoelectronic applications. Electronic struc-
ture for hBN suffer from interlayer interactions and
orbital overlaps. DOS for both systems are calcu-
lated and agree with the analysis of bands in k-
space. Charge transfer between the two layers
indicate the formation of a dipole in the interface,
responsible for shifting band discontinuities and
creating a potential barrier between the two layers.
Thus, interlayer interactions and twists play a role
in slight modulations of the hBN substrate, but
electronic properties of MoSe2 are kept unchanged.
ACKNOWLEDGEMENTS
This work was supported by the Brazilian funding
agencies Conselho Nacional de Desenvolvimento
Cientı́fico e Tecnológico (Grant No. 311060/2013-7),
Fundação de Amparo à Pesquisa do Estado de São
Paulo (Grant No. 2012/50738-3) and Coordenação de
Aperfeiçoamento de Pessoal de Nı́vel Superior
(Programa Professor Visitante do Exterior, Grant
3916
No. 88881.068355/2014-01 and scholarship grant)
within the program Science Without Borders, and
by Instituto Tecnológico de Aeronáutica (ITA) T-61
(alumni supporting ITA). The authors acknowledge
L. Matthes and A. Marques for their useful advice
and prolific discussions.
REFERENCES
1. M. Xu, T. Liang, M. Shi, and H. Chen, Chem. Rev. 113(5),
3766 (2013).
2. C.R. Dean, A.F. Young, I. Meric, C. Lee, L. Wang, S. Sor-
genfrei, K. Watanabe, T. Taniguchi, P. Kim, K. Shepard,
and J. Hone, Nat. Nanotechnol. 5(10), 722 (2010).
3. N. Verbitskiy, A. Fedorov, G. Profeta, A. Stroppa, L.
Petaccia, B. Senkovskiy, A. Nefedov, C. Wöll, D.Y. Usa-
chov, D. Vyalikh, L. Yashina, A. Eliseev, T. Pichler, and A.
Grüneis, Sci. Rep. 5, 17700 (2015).
4. A.S. Mayorov, R.V. Gorbachev, S.V. Morozov, L. Britnell, R.
Jalil, L.A. Ponomarenko, P. Blake, K.S. Novoselov, K.
Watanabe, T. Taniguchi, and A. Geim, Nano Lett. 11(6),
2396 (2011).
5. F. Amet, J. Williams, A. Garcia, M. Yankowitz, K.
Watanabe, T. Taniguchi, and D. Goldhaber-Gordon, Phys.
Rev. B 85(7), 073405 (2012).
6. A. Pakdel, Y. Bando, and D. Golberg, Chem. Soc. Rev. 43(3),
934 (2014).
7. F. Withers, O. Del Pozo-Zamudio, A. Mishchenko, A. Roo-
ney, A. Gholinia, K. Watanabe, T. Taniguchi, S. Haigh, A.
Geim, A. Tartakovskii, and K. Novoselov, Nat. Mater.
14(3), 301 (2015).
8. S.W. King, M.M. Paquette, J.W. Otto, A.N. Caruso, J.
Brockman, J. Bielefeld, M. French, M. Kuhn, and B.
French, Appl. Phys. Lett. 104(10), 102901 (2014).
9. D. Jariwala, V.K. Sangwan, L.J. Lauhon, T.J. Marks, and
M.C. Hersam, ACS Nano 8(2), 1102 (2014).
10. Q.H. Wang, K. Kalantar-Zadeh, A. Kis, J.N. Coleman, and
M.S. Strano, Nat. Nanotechnol. 7(11), 699 (2012).
11. B. Radisavljevic, A. Radenovic, J. Brivio, V. Giacometti,
and A. Kis, Nat. Nanotechnol. 6(3), 147 (2011).
12. Z. Yin, H. Li, H. Li, L. Jiang, Y. Shi, Y. Sun, G. Lu, Q.
Zhang, X. Chen, and H. Zhang, ACS Nano 6(1), 74 (2011).
13. S. Tongay, J. Zhou, C. Ataca, K. Lo, T.S. Matthews, J. Li,
J.C. Grossman, and J. Wu, Nano Lett. 12(11), 5576 (2012).
14. S. Larentis, B. Fallahazad, and E. Tutuc, Appl. Phys. Lett.
101(22), 223104 (2012).
15. S.R. Das, J. Kwon, A. Prakash, C.J. Delker, S. Das, and
D.B. Janes, Appl. Phys. Lett. 106(8), 083507 (2015).
16. A. Geim and I. Grigorieva, Nature 499(7459), 419 (2013).
Koda, Bechstedt, Marques, and Teles
17. S. Dufferwiel, S. Schwarz, F. Withers, A. Trichet, F. Li, M.
Sich, O. Del Pozo-Zamudio, C. Clark, A. Nalitov, D. Sol-
nyshkov, G. Malpuech, K. Novoselov, J. Smith, M. Skol-
nick, D. Krizhanovskii, and A. Tartakovskii, Nat.
Commun. 6, 8579 (2015).
18. F. Withers, O. Del Pozo-Zamudio, S. Schwarz, S. Duffer-
wiel, P. Walker, T. Godde, A.P. Rooney, A. Gholinia, C.
Woods, P. Blake, S. Haigh, K. Watanabe, T. Taniguchi, I.
Aleiner, A. Geim, V. Fal’ko, A. Tartakovskii, and K. No-
voselov, Nano Lett. 15(12), 8223 (2015).
19. C.R. Woods, L. Britnell, A. Eckmann, R.S. Ma, J.C. Lu,
H.M. Guo, X. Lin, G.L. Yu, Y. Cao, R.V. Gorbachev, A.V.
Kretinin, J. Park, L.A. Ponomarenko, M.I. Katsnelson,
Y.N. Gornostyrev, K. Watanabe, T. Taniguchi, C. Casir-
aghi, H.J. Gao, A.K. Geim, and K.S. Novoselov, Nat. Phys.
10(6), 451 (2014).
20. Y. Shi, W. Zhou, A.Y. Lu, W. Fang, Y.H. Lee, A.L. Hsu,
S.M. Kim, K.K. Kim, H.Y. Yang, L.J. Li, J.C. Idrobo, and J.
Kong, Nano Lett. 12(6), 2784 (2012).
21. W. Kohn and L.J. Sham, Phys. Rev. 140(4A), A1133 (1965).
22. H. Kumar, L. Dong, and V.B. Shenoy, Sci. Rep. 5, 21516
(2016).
23. Y. He, Y. Yang, Z. Zhang, Y. Gong, W. Zhou, Z. Hu, G. Ye,
X. Zhang, E. Bianco, S. Lei, Z. Jin, X. Zou, Y. Yang, Y.
Zhang, E. Xie, J. Lou, B. Yakobson, R. Vajtal, B. Li, and P.
Ajayan, Nano Lett. 16(5), 3314 (2016).
24. D.S. Koda, F. Bechstedt, M. Marques, and L.K. Teles, J.
Phys. Chem. C 120, 10895 (2016).
25. G. Kresse and J. Furthmüller, Comput. Mater. Sci. 6, 15
(1996).
26. G. Kresse and J. Furthmüller, Phys. Rev. B 54, 11169
(1996).
27. P.E. Blöchl, Phys. Rev. B 50, 17953 (1994).
28. G. Kresse and D. Joubert, Phys. Rev. B 59, 1758 (1999).
29. J.P. Perdew, K. Burke, and M. Ernzerhof, Phys. Rev. Lett.
77(18), 3865 (1996).
30. J. Klimeš, D.R. Bowler, and A. Michaelides, Phys. Rev. B
83(19), 195131 (2011).
31. H.J. Monkhorst and J.D. Pack, Phys. Rev. B 13(12), 5188
(1976).
32. P.E. Blöchl, O. Jepsen, and O.K. Andersen, Phys. Rev. B
49(23), 16223 (1994).
33. K. Momma and F. Izumi, J. Appl. Crystallogr. 41(3), 653
(2008).
34. D.M. Guzman and A. Strachan, J. Appl. Phys. 115(24),
243701 (2014).
35. T. Björkman, A. Gulans, A.V. Krasheninnikov, and R.M.
Nieminen, Phys. Rev. Lett. 108(23), 235502 (2012).
36. N. Ashcroft and N. Mermin, Solid State Physics (Thomson
Learning, South Melbourne, 1976).