International Journal of Heat and Mass Transfer 137 (2019) 161–173

Contents lists available at ScienceDirect

International Journal of Heat and Mass Transfer

journal homepage: www.elsevier.com/locate/ijhmt

How interlayer twist angles affect in-plane and cross-plane thermal

conduction of multilayer graphene: A non-equilibrium molecular
dynamics study
Xianhua Nie, Li Zhao ⇑, Shuai Deng, Yue Zhang, Zhenyu Du
Key Laboratory of Efficient Utilization of Low and Medium Grade Energy (Tianjin University), MOE, Tianjin University, Tianjin 300350, China

a r t i c l e i n f o a b s t r a c t

Article history: Graphene, a kind of emerging low dimensional carbon material, has admirable thermal properties with
Received 4 January 2019 potential applications in the thermal management of aerospace and microelectronics fields. In recent
Received in revised form 19 March 2019 studies, thermal properties of both conventional single-layer and multilayer graphene were extensively
Accepted 22 March 2019
studied. However, few studies focused on that of multilayer graphene with twist angles, whose thermal
Available online 26 March 2019
properties are different from that of conventional graphene because of the existence of interlayer twist
angles. Such knowledge gap hinders the potential applications. Therefore, the thermal conductivity of
Keywords:
bilayer, 4-layers and 6-layer zigzag graphene with various twist angles is investigated utilizing non-
Multilayer graphene
Twist angle
equilibrium molecular dynamics at the typical temperature region in this study, and both in- and
In-plane thermal conduction cross-plane thermal conductivity are investigated. The size of the studied graphene is 10 nm
22 nm
Cross-plane thermal conduction in the x-y plane, and the size in the z-direction depends on the number of layers. Moreover, the phonon
Non-equilibrium molecular dynamics vibrational density of state is also analyzed for mechanisms behind the thermal transport. The result indi-
cates that a local maximum value can be found with the twist angle of 30° for in-plane thermal conduc-
tion. The results also suggest that the highest thermal conductivity could be reached without any twist
angles for both in and cross-plane conduction. The observation would provide an opportunity to study
the characteristics of in-plane and cross-plane thermal transport of twisted multilayer graphene.
Ó 2019 Elsevier Ltd. All rights reserved.

1. Introduction
Carbon material, particularly graphene, is the promising ther-
mal dissipating material in aerospace and microelectronics appli-
cations, due to their unique characteristics of thermal transport.
Several studies indicated that the thermal conductivity of gra-
phene exceeds that of some other materials. For instance, thermal
conductivity of graphene (2000 W/mK) is five orders of magni-
tude larger than that of amorphous carbon (0.01 W/mK), five
times larger than that of metals (400 W/mK) and even twice lar-
ger than that of polycrystalline diamond (1000 W/mK) [1–3].
Consequently, there are increasing experimental and theoretical
studies focusing on the thermal transport in graphene nowadays,
particularly on a quantized index of thermal conductivity.
Direct understanding on thermal properties of graphene origi-
nates from experiments and plenty of researchers measured the
thermal conductivity of graphene [4–9]. Balandin et al. measured
the thermal conductivity of suspended single layer graphene utiliz-
⇑ Corresponding author.
E-mail address: jons@tju.edu.cn (L. Zhao).
ing an original Raman optothermal method. It was found that the
thermal conductivity of single layer graphene near room tempera-
ture is in the range from 2000 W/mK to 5300 W/mK, depending
on the sample size and quality [4–6]. Cai et al. [7] studied the ther-
mal transport of suspended single-layer graphene grown by chem-
ical vapor deposition, and a thermal conductivity of about 2500 W/
mK was obtained utilizing Raman optothermal at 350 K. Besides of
studies on suspended graphene, Seol et al. [8] measured the ther-
mal conductivity of supported single-layer graphene utilizing elec-
trical method, and the value is about 600 W/mK. They found that
compared to that of suspended graphene, the thermal conductivity
of supported graphene decreases because of the loss of phonon
energy across the graphene-support interface. However, although
the experiment is considered as the most reliable method, there’re
still some limitations. Firstly, the quality of graphene is a vital fac-
tor for the accuracy of experiments, but the quality of graphene
produced in the world is still poor nowadays [10], and a survey
revealed that a plenty of researches on graphene could be under-
mined by the poor quality of available graphene [11]. Therefore,
there would be expensive for a high-quality graphene, and it is nei-
ther convenient nor economy to conduct experiments on a large

https://doi.org/10.1016/j.ijheatmasstransfer.2019.03.130
0017-9310/Ó 2019 Elsevier Ltd. All rights reserved.
162 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173
number of samples. Secondly, some complex structures of multi-
layer graphene cannot be obtained based on existing technical con-
ditions. What’s more, the mechanism of thermal transport from
the phonon point of view could not be directly revealed by exper-
iments, and it has become a main barrier to understand the ther-
mal transport phenomena or behavior inside graphene.
Facing limitations of current experimental studies, theoretical
modeling such as Boltzmann transport equation [8,12,13], and
molecular dynamics (MD) simulation provides powerful tools to
model the phonon transport of materials [14–16]. For Boltzmann
transport equation, the phonon-dispersion curves should be deter-
mined in advance, but it would be difficult to be determined in
some conditions, especially when the studied graphene is not ideal
and suspended [17]. Therefore, MD, especially non-equilibrium
molecular dynamics (NEMD), is widely considered as a promising
approach to refine the existing research framework, and the ther-
mal transport can be characterized once the intermolecular inter-
actions are determined. Table 1 shows a brief state of the art of
MD studies on graphene’s thermal transport. Because of the aniso-
tropy of graphene, both in-plane and cross-plane thermal conduc-
tivity should be investigated separately. For in-plane conduction,
Bazrafshan et al. [14] studied the single layer amorphous graphene
utilizing NEMD, and the effects of the defect concentration, defect
distribution and strain were analyzed. Xu et al. [18] proposed a
study on the effects of length and temperature on thermal conduc-
tivity of single layer graphene through experiments and NEMD. In
this research, thermal conductivity obtained by NEMD agrees well
with experimental data, furthermore, mechanisms of thermal con-
duction from phonon point of view were also revealed by NEMD.
For cross-plane condition, the cross-plane thermal resistances of
graphene/water interface [19,20], graphene/metal interface [21]
and graphene/MoS2 interface [15] are the focuses. However, as dis-
cussed above and in Table 1, compared to studies on in-plane ther-
mal transport, there’s little study focusing on the cross-plane
thermal transport of the graphene/graphene interface. Thus, this
is still a knowledge gap remaining to be solved.
Furthermore, in recent studies, Cao et al. [24,25] discovered a
unique phenomenon of multilayer graphene’s electronic proper-
ties. When there’s an interlayer twist angle of 1.1°, named ‘‘magic
angle”, existing between layers, Mott-like insulator can be
obtained [24]. Furthermore, based on these structures, when
there’re some electrical carriers, an unconventional superconduc-
Table 1
State-of-the-art of MD studies on thermal transport in graphene samples.
Heat Flux Year Type of graphene Size of samples
[Ref.]
In-plane 2017 Single layer; 17 nm
5 nm;
[17] multilayer 50 nm
5 nm
2014 Single layer The longest length is
[18] 9 lm
2012 Single layer (20–2800)
[22] nm
5.2 nm
2011 Multilayer 7–25 nm in length
[23]
Cross-plane 2016 Multilayer/MoS2 The number of
[15] graphene is 7
2015 Multilayer/metal The number of
[21] graphene
ranges from 1 to 5
tivity of bilayer graphene appears [25]. Furthermore, Yankowitz
et al. [26] found that the superconductivity can also be found with
the twist angle larger than 1.1°. These studies make the twisted
multilayer graphene be a hot topic. However, what would be the
phenomenon for thermal transport, and does the twist angles have
a significant effect on thermal conduction of multilayer graphene?
As for experimental studies [27,28], as discussed above, the twist
angle is difficult to be controlled to an exact angle. As for some
MD studies, Hu et al. [29] studied the effect of chirality degree
on thermal conductivity of single layer graphene and eight chiral-
ity degrees were evaluated. Cocemasov et al. [30,31] and Li et al.
[32] carefully studied the mechanism of phonon transport in
twisted bilayer graphene, and the effect of out-of-plane phonon
modes on thermal conduction were comprehensively analyzed.
These studies mainly focus on the in-plane thermal transport of
twisted bilayer graphene, because the deep mechanism analyses
can be conveniently revealed based on a simple configuration of
graphene. However, not only bilayer graphene and in-plane con-
duction, but also multilayer graphene and cross-plane conduction
have a broad application. To the best of the authors’ knowledge,
the systematic study on the changes of the thermal conductivity
of multilayer graphene with a series of twist angles are rarely
reported in published studies. What’s more, the effect of the twist
angle on cross-plane conduction is also limited. Therefore, all of
these knowledge gaps should be further studied.
In this work, the effect of the interlayer twist angle on the ther-
mal conductivity of multilayer graphene are investigated utilizing
NEMD, and both thermal conductivity of in-plane conduction and
interfacial conductance of cross-plane conduction are considered.
In NEMD, the twist angles (0°, 1°, 5°, 10°, 20°, 30°, 40°, 50°, 55°
and 59°) together with their positions, the number of layers
(bilayer, 4-layer and 6-layer), direction of heat flux (in-plane and
cross-plane) and temperatures (from 200 K to 600 K) are all evalu-
ated. Besides, the mechanism behind the thermal conduction is
further analyzed with the help of the vibrational density of state
(VDOS). To the best of the authors’ knowledge, this study is one
of the few comprehensive and systematic MD studies and analyses
on thermal conductivity of multilayer graphene with twist angles
(MGTA) compared with existing studies. Particularly, this study
explores a relationship between interlayer twist angles and ther-
mal conductivity. For further conclusion, thermal properties would
significantly deteriorate if the structure of multilayer graphene
Range of Maximum value Descriptions
Temperature
200–500 K 423 W(mK)1; Evaluate the performance of various
As shown in Fig. 7(a) in potential utilized in MD
Ref. [17]
100–1000 K 2307 W(mK)1; Discover the effect of length on thermal
As shown in Fig. 3b in Ref. conductivity of suspended graphene
[18] experimentally, and the results are
compared by MD
100–1000 K 2360 W(mK)1; Study the conduction of graphene
As shown in Fig. 3 in Ref.
[22]
300 K–800 K 870 W(mK)1; Evaluate the effect of the number of layers
As shown in Fig. 4 in Ref. on thermal conductivity. Nevertheless, the
[23] results weren’t corrected by quantum
effect
300 K 213 MW(m2K)1; Calculated the interfacial thermal
As shown in Table 2 in conductance of graphene/MoS2
Ref. [15] heterostructures.
– – Calculated the interfacial thermal
conductance of graphene/metal interface
 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173 163

deviates the designed configuration. Above all, this study can pro-
vide a guided tour to the effect of the twist angle on thermal trans-
port of graphene, and it benefits to the regulation of the thermal
conductivity of the multilayer graphene for potential thermal man-
agement in microelectronics and aerospace.

2. Simulation methods

In this study, all of the simulations were performed with the

Large-scale Atomic/Molecular Massively Parallel Simulator
(LAMMPS) package [33], and atom visualization was done by Open
Visualization Tool (OVITO) [34]. The range of temperature in the
study is from 200 K to 600 K with a step of 100 K, which is a typical
temperature range in current studies as shown in Table 1. The time
step of the simulation was set as 1 fs. Schematic diagram of MGTA
can be seen in Fig. 1 (taking 6-layer graphene as an example), and
the initial chirality of graphene is zigzag graphene. The length in
x-direction is 22 nm while the length in y-direction is 10 nm. In
addition, the distance between two adjacent layers in z-direction
is 0.35 nm, thus the complete length of the multilayer graphene
in z-direction is 0.35n nm, where n represents the number of layers.
Fig. 2 shows configurations and local enlarged structures of
MGTA. In this study, twist angles of 0° (without interlayer twist
angle), 1°, 5°, 10°, 20°, 30°, 40°, 50°, 55°, and 59° are investigated.
Because of the symmetry of hexagon, configurations with twist
angles of 40°, 50°, 55°, and 59° are the same as that of 1°, 5°, 10°,
20°, thus only angles of 1–30° are demonstrated in Fig. 2(b)–(f). Fur-
thermore, in order to evaluate the effect of the position where the
twist angles exist, different positions of the twist angle are also
established respectively. For the 4-layer MGTA, the twist angles
exist between the first and the second layers, and between the sec-
ond and the third layers, while for the 6-layer MGTA, the twist angles
exist between the first and the second layers, between the second
and the third layers, and between the third and the forth layers.
The optimized Tersoff potential (opt-Tersoff), which has been
proved to be the most suitable potential for thermal transport
modeling of the graphene [17,35], was utilized to describe the
Fig. 1. Schematic diagram of MGTA and NEMD model (Taking 6-layer MGTA as an
intra-layer sp2 interactions. In addition, Lennard-Jones (LJ) poten- example). (a) Configuration and the size of the MGTA; (b) NEMD model with
tial as shown in Eq. (1), whose parameters are obtained from Gir- simplified scales of in-plane conduction; (c) NEMD model with simplified scales of
ifalco et al. [36], was utilized to model the van der Waals cross-plane conduction.
interaction among different layers. Moreover, the temperature T
of the graphene was calculated according to the average kinetic
kq dT MD
energy of all atoms in the layer and it can be seen in Eq. (2). Where ¼ ð4Þ
N is the number of atoms; kB is the Boltzmann constant; m repre- kMD dT q
sents the mass of atoms, and p represents the momentum of atoms. For in-plane conduction, the schematic model can be seen in
However, the temperature calculated by MD is based on the Debye Fig. 1(b). As shown in Fig. 1(b), the size of the studied MGTA is
assumption, and it is suitable for the condition where tempera- 22 nm
10 nm in the x-y plane, and the size in z-direction is deter-
tures are higher than the Debye temperature. In this study, tem- mined by the number of layers with a premise that the distance
peratures of graphene are far lower than 2100 K (Debye between adjacent layers is 0.34 nm. Besides, in order to create
temperature of the graphene), thus quantum correction must be the temperature gradient, heat source and heat sink are estab-
introduced. The expression of quantum correction can be seen in lished, and they’re colored in red and blue respectively. Non-
Eqs. (3) and (4) [22,37,38]. Where TMD represents the temperature periodic boundaries (shrink-wrapped boundary condition) are per-
calculated by MD; Tq represents the quantum corrected tempera- formed for x, y and z directions. Firstly, in order to avoid the
ture; x represents the angular frequency of phonons; xD repre- dynamic re-orientation of twist angles, both sides of the studied
sents the Debye frequency. configuration were fixed to restrain the re-orientation during
"

6 #
r12
r MD. During the simulation of in-plane conduction, the simulation
uLJ ¼ 4e  ð1Þ box was initially relaxed in microcanonical (NVE) ensemble for
r ij r ij
100 ps, which is enough to reach an initial equilibrium. Then, the
region with a width of 0.5 nm on both sides of the MGTA was fixed,
2 X p2i
T MD ¼ ð2Þ and next to the fixed region, there’re heat source and heat sink
3NkB i 2mi with constant temperatures controlled by Langevin thermostats.
! Followed by which, another 5 ns in NVE ensemble was processed
Z xmax
9N 1 1 in order to reach a satisfactory linear temperature profile. A typical
3NkB T MDi ¼ x
2
þ hxdx
— ð3Þ
0 x3D hx
—
ekB T q 1 2
temperature profile of the MGTA can be seen in Fig. 3(a), and only
the linear region (red line in Fig. 3) was utilized to calculate the
164 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173
Fig. 2. Schematic diagram and enlarged structures of MGTA. (a) The twist angle is 0°; (b) The twist angle is 1°; (c) The twist angle is 5°; (d) The twist angle is 10°; (e) The twist
angle is 20°; (f) The twist angle is 30°.
temperature gradient in this study. Then, the Fourier’s law, as
shown in Eq. (5), was implemented to calculate the in-plane ther-
mal conductivity.
@T
q ¼ kA
@x
For cross-plane conduction, the schematic model can be seen in
Fig. 1(c). Similar to the procedure of in-plane conduction, the heat
source and heat sink were also created to generate the temperature
gradient. Different from the in-plane conduction simulation, for
the study on cross-plane conduction of 6-layer MGTA, the initial
configuration of 8-layer should be established, and the top and bot-
tom layers of the multilayer graphene were set as the heat source
and heat sink respectively. Moreover, because the cross-plane ther-
mal conductivity is lower than in-plane conductivity, therefore,
10 ns in the NVE ensemble was processed for cross-plane conduc-
tion in order to reach a good equilibrium of temperature profile. A
typical temperature profile of cross-plane conduction can be seen
in Fig. 3(b). As shown in the figure, the relationship between the
position and temperatures are not linear, and there’s a sudden
temperature decrease DT at the position where the twist angle
exists. Therefore, interfacial thermal conductance replace the ther-
mal conductivity to characterize the cross-plane thermal transport.
The calculation of the interfacial thermal conductance can be seen
in Eq. (6). Where R represents the interfacial thermal conductance
with a unit of MW/(m2K).
q temperature increases to 300 K, the thermal conductivity
R¼
ADT
3. Results analyses
3.1. In-plane thermal conductivity
ð5Þ 3.1.1. Effects of twist angles and the number of layers at different
temperatures
The in-plane thermal conductivity of the bilayer, 4-layer, and 6-
layer MGTA at different temperatures can be seen in Fig. 4(a)–(c)
respectively. For the convenience of comparison, all of the results
shown in Fig. 4 are based on the configuration with twist angles
existing in the middle of the MGTA (between the first and the sec-
ond layers of bilayer MGTA, between the second and the third lay-
ers of 4-layer MGTA, between the third and the forth layer of 6-
layer MGTA). In each figure, the horizontal axis represents the tem-
perature, while the vertical axis represents the in-plane thermal
conductivity. Meanwhile, the solid lines represent results derived
by NEMD, while the dash lines represent the quantum corrected
results. Moreover, considering the symmetry of hexagon, only
twist angles ranging from 0° to 30° are demonstrated in the figures
for a clear description.
It can be seen that the trends of NEMD and quantum corrected
results are different. For all of the results calculated by NEMD, in-
plane thermal conductivity decreases as temperatures increase, no
matter what the twist angle is. For instance, as can be seen in solid
lines of Fig. 4(a), the thermal conductivity of bilayer MGTA with
the interlayer twist angle of 0° at 200 K is 648 W/mK, and as the
ð6Þ
decreases to 529 W/mK. Furthermore, when the temperature con-
 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173 165

Fig. 3. Temperature profiles of in-plane and cross-plane conduction. (a) A typical

steady temperature profile of in-plane conduction with 100 segments in x-
direction; (b) Typical temperature profile of cross-plane conduction in z-direction
(taking 6-layer MGTA as an example).

tinues to increase, the thermal conductivity decreases correspond-

ingly. Besides, the MGTA with other twist angles has the similar
regulation. However, for results obtained by the quantum correc-
tion, the thermal conductivity increases firstly and decrease subse-
quently as the temperature increases. The crossover temperature is
about 320 K. This crossover point results from the Umklapp pho-
non scattering [22]. Therefore, the results obtained by Eq. (2) lead
to an inaccurate estimation of the thermal conductivity, especially
in the low temperature region, and the quantum corrected thermal
conductivity should be utilized for analyses.
In order to evaluate the effects of the temperature, the twist
angle and the number of layers on in-plane thermal conductivity
in an intuitive way, results are demonstrated in Fig. 5(a). Moreover,
different views of Fig. 5(a) can also be seen in Fig. 5(b) and (c). Only
quantum corrected results are presented in the figure. In the figure,
the left axis of the horizontal plane represents the number of lay-
ers, thus the three groups of curves in the figure represent the ther- Fig. 4. Relationship between temperatures and in-plane thermal conductivity of
mal conductivity of bilayer, 4-layer, and 6-layer MGTA. The right MGTA (10 nm
22 nm in the x-y plane) with different twist angles. (a) Bilayer
axis of the horizontal plane represents the twist angle. Although MGTA; (b) 4-layer MGTA; (c) 6-layer MGTA.
166 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173
the MGTA have configuration symmetry during torsion, MGTA
with all of the twist angles are calculated in order to evaluate if
the symmetry has some effects on thermal conductivity. In addi-
tion, different colors of curves represent different temperatures.
The following conclusions can be obtained according to Fig. 5:
Firstly, MGTA with the symmetric twist angles of a hexagon
have the same thermal conductivity. Taking bilayer MGTA at
600 K as an example, thermal conductivity of the MGTA with twist
angle of 20° is 242 W/mK, while which with twist angle of 40° is
242 W/mK, and other symmetric twist angles such as 10° and
50°, 5° and 55° etc. lead to the same conclusion. That’s why the
shape of curves is ‘‘W-shaped”.
Secondly, for each MGTA, in the range of 0–10°, a slight twist
angle can lead to a significant decrease in thermal conductivity.
The thermal conductivity of bilayer, 4-layer, and 6-layer MGTA
without any twist angles is 329 W/mK, 219 W/mK and 199 W/
mK respectively at 600 K. However, when there’s a slight twist
angle, such as 1°, thermal conductivity decreases by 9.38%, 8.80%,
10.32% and reach 298 W/mK, 200 W/mK and 178 W/mK respec-
tively. As twist angles further increase to the range of 10–20°,
the decrease rate of thermal conductivity becomes smaller than
that in the range of 0–10°. However, when the twist angle further
increases to 30°, the angle where the twisted layer becomes arm-
chair graphene, the thermal conductivity have a significant
increase and becomes a local maximum value. However, the ther-
mal conductivity at this point is still lower than that of the MGTA
without any twist angles. The maximum values at 600 K for
bilayer, 4-layer, and 6-layer MGTA are 286 W/mK, 183 W/mK
and 164 W/mK respectively.
Thirdly, the effect of the number of layers on the in-plane ther-
mal conductivity can also be illustrated in Fig. 5(c). Intuitively, a
large number of layers leads to a lower thermal conductivity. At
600 K, the thermal conductivity is 329 W/mK, 219 W/mK and
199 W/mK for bilayer, 4-layer, and 6-layer MGTA respectively
without twist angles. Moreover, as the number of layers increases
from 2 to 4, the thermal conductivity decreases by 33.40%, and as
the number of layers increases from 4 to 6, it further decreases by
9.36%. It can be seen that the decrease rate of thermal conductivity
is lower and lower as the number of layers increases. Results
obtained from the other twist angles and temperatures lead to a
similar conclusion. Furthermore, based on the analyses, there’s
assumed to be a critical number of layers, above which the thermal
conductivity would not be changed as the number of layers.
Above all, the effects of the temperatures, the twist angles and
the number of layers on in-plane thermal conductivity are con-
cluded. However, only configurations with twist angles existing
in the middle of MGTA are analyzed in Figs. 4 and 5, if the position
of twist angles affects the thermal conductivity should be further
studied. Therefore, additional simulations were also conducted in
order to find out the effect of the twist angles’ position on the ther-
mal conductivity, and the results can be seen in Fig. 6. Fig. 6(a) is
for 6-layer MGTA and all possible positions where twist angles
can exist are discussed. As for 6-layer MGTA, there’re three possi-
ble positions. The twist angle can exist between the first and the
second layers (shown by dot lines), the second and the third layers
(shown by dash-dot lines), as well as the third and the fourth lay-
ers (shown by solid lines). Fig. 6(b) shows similar information of 4-
layer MGTA and the only difference is that the twist angle can only
exist between the first and the second layers (shown by dash-dot
lines) and between the second and the third layers (shown by solid
lines). In Fig. 6, only quantum corrected results are demonstrated
and different colors represent different twist angles.
It can be seen in Fig. 6, the position of twist angles is also a vital
factor affects thermal conductivity. For example, as for 6-layer
MGTA with the twist angle of 1° at 300 K, the thermal conductivity
is 225 W/mK when the twist angle exists between the third and
the fourth layers. When the twist angle exists between the second
and the third layers, the thermal conductivity is 213 W/mK,
decreased by 5.63%. Meanwhile, when the twist angle exists
between the first and the second layers, the thermal conductivity
is 201 W/mK, further decreased by 5.34%. This means that in-
plane conductivity depends on the difference between the num-
bers of layers on both sides of the twist angle, and the larger the
difference is, the lower the in-plane thermal conductivity is. That
is to say, when the twist angle exists between the third and the
forth layers for 6-layer MGTA, the difference is 0, and the highest
thermal conductivity among the three configurations with 1° twist
angle can be obtained. Moreover, when the twist angle exists
between the second and the third layers, the difference is 1, and
the thermal conductivity decreases.
3.1.2. In-plane thermal conduction from phonon point of view
In order to understand the thermal conduction on nanoscale,
characteristics of phonons during thermal conduction should be
considered, and it can be quantified by VDOS. The calculation of
VDOS can be seen in Eq. (7), which is a Fourier transformation of
the velocity autocorrelation function (VACF) as shown in Eq. (8).
In general, the low-frequency phonons play a significant role in
the thermal conduction. Particularly, phonons with the frequency
lower than 20THz dominate the thermal conductivity [39].
Z s
VDOSðxÞ ¼ VACF ðtÞe2pixt dt ð7Þ
0
P 
v i ð0Þv i ðtÞ 
VACF ðt Þ ¼ P i ð8Þ
i v i ð0Þv i ð0Þ
In order to understand the effect of twist angles on in-plane
thermal conduction from phonon point of view, Fig. 7, which
demonstrates the VDOSs of 4-layer MGTA at 400 K, are presented.
Because the heat flux is in the x-direction for in-plane thermal con-
duction, thus it only shows the phonon oscillation in the x-
direction. In addition, VDOSs of 4-layer MGTA with twist angles
of 0°, 10°, and 30° are compared in Fig. 7(a). Moreover, the his-
togram of frequency distribution with an interval of 20 THz, which
represents the proportion of phonons in different frequency inter-
vals, is presented in Fig. 7(b) in order to give a clear description of
the distribution of phonons. Therefore, the effect of twist angles on
in-plane thermal conductivity can be explained from the following
two aspects:
Firstly, the interlayer twist angles affect the distribution of low-
frequency phonons. It can be seen in Fig. 7(a), for 4-layer MGTA
with different twist angles, the VDOSs are similar to each other.
There’re apparent peaks at the frequency of 49 THz approximately
for the three configurations. This indicates that the existence of
twist angles have a slight effect, or even no effects, on the peak
of VDOSs. Furthermore, it can be seen in Fig. 7(b), MGTA with
the twist angle of 10° has the smallest proportion of phonons in
the interval of 0–40 THz compared to the MGTA with twist angles
of 0° and 30°, and that’s why the 4-layer MGTA with twist angle of
10° has the lowest in-plane thermal conductivity among these
three configurations. As for MGTA with twist angles of 0° and
30°, the proportions of phonons in the interval of 0–40 THz are
approximately the same. Nevertheless, in the interval of 40–60
THz, the proportion of phonons for MGTA with a twist angle of
0° is higher than that of 30°, especially in the range of 40–50
THz. Therefore, the in-plane thermal conductivity of MGTA with
the twist angle of 0° (Zigzag/ Zigzag) is higher than that of MGTA
with the twist angle of 30° (Armchair/ Zigzag).
Secondly, the roughness of the edge perpendicular to the direc-
tion of heat flux can also affect the in-plane thermal conduction
[29], and the edge of graphene (colored in red) with different twist
 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173 167

Fig. 5. In-plane thermal conductivity of MGTA (10 nm
22 nm in the x-y plane) with different numbers of layers, twist angles and temperatures. (a) Global figure of
relationship among the thermal conductivity, the twist angle and the number of layers. (b) Thermal conductivity - twist angle view of the global figure (taking temperature of
400 K as an example). (c) Thermal conductivity – the number of layers view of the global figure (taking the twist angles of 0° and 30°, the temperature of 400 K as an
example).

angles can be seen in Fig. 8. A rough edge results in the increase of
the number of scattering centers in the configuration, and this
causes the enhancement the phonon scattering and the reduction
of the mean free path of phonons. These factors lead to low con-
ductivity eventually. In current studies, it’s widely considered that
the zigzag graphene has the smoothest edge and the armchair gra-
phene has the relatively smooth edge. Furthermore, the increase of
twist angle between 0° and 30° results in the increase of edge
roughness.
Besides, to study the effect of the number of layers on in-plane
thermal conductivity from phonon point of view, comparison of
the proportion of low-frequency phonons between bilayer and 4-
layer MGTA can be seen in Fig. 9. Fig. 9(a) shows the comparison
of bilayer and 4-layer MGTA without twist angles, while Fig. 9(b)
shows the comparison of bilayer and 4-layer MGTA with a twist
angle of 10°. From Fig. 9(a), it can be seen that in the interval of
0–20 THz, the proportions of phonons of 4-layer and bilayer MGTA
are approximately the same. The value of the former one is 21.92%,
168 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173

Fig. 7. Comparison of VDOS in x-direction of 4-layer MGTA with twist angles of 0°,
10°, and 30°. (a) VDOS; (b) The histogram of frequency distribution of phonons.

Fig. 6. The effect of the position where the twist angle exists on thermal
conductivity at different temperatures. (a) For 6-layer MGTA whose twist angles the difference between the numbers of layers on both side
exist between the first and the second, the second and the third, the third and the increase. It can also be concluded that the reduction rate of the
forth layers respectively; (b) For 4-layer MGTA whose twist angles exist between
the first and the second, the second and the third layers respectively.
thermal conductivity caused by the increase in the number of lay-
ers is larger, compared to the increase rate of the thermal conduc-
tivity caused by the reduction of the number of layers.
and that of the latter one is 22.00%. However, in the interval of 20–
40 THz, the proportion of phonons of bilayer MGTA is apparently
3.2. Cross-plane thermal conductivity
higher than that of 4-layer MGTA. As for Fig. 9(b), the only appar-
ent difference between the bilayer and 4-layer MGTA can be found
3.2.1. Effects of twist angles and the number of layers at different
in the range of 0–20 THz, as highlighted by the red rectangle.
temperatures
Therefore, for in-plane thermal conduction and VDOS in x-
The cross-plane thermal conduction has different characteris-
direction, the increase in the number of layers results in the reduc-
tics compared to the in-plane conduction, and the effects of the
tion in phonons with low frequencies. This is because the increase
number of layers and temperatures on the cross-plane thermal
in the number of layers limits the excitation of phonon with low
conductivity of MGTA without twist angles can be seen in
frequency in each layer, and leads to a reduction in the thermal
Fig. 10. Moreover, both results calculated by NEMD (dash line)
conductivity.
and quantum corrected (solid line) are presented. It should be
As for the effect of positions of the twist angle on in-plane ther-
noted that the thermal conductivity of the bilayer MGTA was not
mal conductivity, the combination of the effects of the twist angles
considered in Fig. 10, because the number of temperature data is
and the number of layers can be considered as one of the explana-
not enough to obtain a convincing temperature gradient. According
tions. Moreover, if the numbers of layers are not equal on the both
to the figure, it can be seen that:
side of the twist angle, there must be a larger number of layers on
Firstly, the cross-plane thermal conductivity is much smaller
one side and a smaller number of layers on the other side. As dis-
than the in-plane thermal conductivity, and the cross-plane ther-
cussed above, this leads to an increase in the thermal conductivity
mal conductivity is smaller than the in-plane thermal conductivity
of one side and a reduction of the other side. According to the
by about three orders of magnitude. This stems from the fact that
results presented in Fig. 6, the thermal conductivity decreases as
compared to sp2 interaction in a layer, the LJ interaction between
 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173
Fig. 8. Edges of MGTA perpendicular to the direction of the heat flux. (a) MGTA with
a twist angle of 0°; (b) MGTA with a twist angle of 10°; (c) MGTA with a twist angle
of 30°.
layers is not conductive to the thermal conduction. In addition, the
existence of an interface between layers also leads to a scattering
of the phonon energy, thus non-ballistic transport of phonon result
in a low conductivity. Secondly, the relationship between the
cross-plane thermal conductivity and temperatures is similar to
the relationship between the in-plane thermal conductivity and
temperatures. For NEMD results, thermal conductivity decreases
monotonically as temperatures increases, and for quantum cor-
rected results, thermal conductivity increases firstly and then
decrease. The temperature where the crossover appears at about
320 K. Thirdly, different from the in-plane thermal conductivity
169
Fig. 9. The histogram of frequency distribution of phonons in x-direction for bilayer
and 4-layer MGTA. (a) Comparison between bilayer and 4-layer MGTA without
twist angles; (b) Comparison between bilayer and 4-layer MGTA with a twist angle
of 10°.
as shown in Fig. 5, the cross-plane thermal conductivity increases
as the number of layers increases, and this agrees with the results
conducted by Wei et al. [40]. As shown in Fig. 10, lines representing
the cross-plane thermal conductivity of 6-layer MGTA are always
above lines representing that of the 4-layer MGTA. The mechanism
behind the phenomenon will be discussed from the phonon point
of view in Section 3.2.2.
Except for the study of the cross-plane thermal conductivity of
MGTA without twist angles, the effect of the twist angles on cross-
plane thermal conductivity are also investigated. The interfacial
thermal conductance is utilized to characterize the thermal con-
duction across layers. Results for the 6-layer MGTA are shown in
Fig. 11. It can be seen that the interfacial thermal conductance
increases as temperature increases. For NEMD results, the relation-
ship between interfacial thermal conductance and temperature is
linear approximately. For configurations with different twist
angles, the curves are parallel. This indicates that for MGTA with
different twist angles, the growth rate of the interfacial conduc-
tance is approximately the same as the temperature increases.
Nevertheless, for quantum corrected results, the interfacial ther-
170 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173
Fig. 10. Comparison of cross-plane thermal conductivity between the 4-layer and
6-layer MGTA without twist angles (graphene).
mal conductance increases at a larger growth rate at temperatures
lower than about 320 K, while the growth rate becomes smaller
when temperatures higher than 320 K. This is because, at lower
temperatures, the quantum effect results in a large deviation
between NEMD and quantum correlation results.
The effect of twist angles on interfacial thermal conductance
can be seen in Fig. 12 in a more intuitive way, and only quantum
corrected results are presented. Different colors mean different
temperatures. In addition, as validated in Fig. 5, the symmetric
configuration leads to the same thermal conductivity, thus interfa-
cial thermal conductance in the range of 30–59° is obtained by
symmetry according to results in the range of 1–30°, and they
are presented by dash lines.
The relationship between the interfacial thermal conductance
and the twist angle is different from that between the in-plane
thermal conductivity and the twist angle. It can be seen that the
interfacial thermal conductance decreases monotonically when
the twist angle increases from 0° to 30°. The figure can be divided
into three regions. In the range of 1–10°, the interfacial thermal
conductance decreases as the twist angle increases. In this region,
the absolute value of the slope is relatively large, which indicates
Fig. 11. The relationship between the temperature and the cross-plane interfacial
conductance of the 6-layer MGTA with different twist angles.
that a small twist angle leads to a large decrease of interfacial ther-
mal conductance. In the range of 10–20°, the interfacial thermal
conductance continues to decrease, but it has a smaller absolute
value of the slope. In these regions, results are in agreement with
results concluded from Fig. 5. Furthermore, when the twist angle
increases to 30°, the interfacial thermal conductance further
decreases, and becomes a local minimum value, rather than a local
maximum value as indicated in Fig. 5.
3.2.2. Cross-plane thermal conduction from phonon point of view
The direction of heat flux is in z-direction for cross-plane con-
duction, thus VDOS in the z-direction as shown in Figs. 13 and
14 are selected to study the cross-plane thermal conduction.
To understand the effect of the number of layers on cross-plane
thermal conductivity, a comparison between VDOSs of 4-layer and
6-layer MGTA is presented in Fig. 13(a) and the corresponding pro-
portion of phonons in different frequency intervals can be seen in
Fig. 13(b). It can be seen that the number of layers has a slight
effect on the peak of VODSs, and for both configurations, apparent
peaks exist at frequencies of about 13 THz and 26 THz. Neverthe-
less, the proportions of phonons in different frequency intervals
are different, and these differences result in the difference of
cross-plane thermal conductivity. In the interval of 0–20 THz, the
proportion of phonons for 6-layer MGTA is higher than that for
4-layer MGTA, and the former value is 50.66%, while the later
one is 49.36%. Furthermore, although the proportion of phonons
for 6-layer MGTA is lower than that for 4-layer MGTA in the range
of 20–40 THz, the difference (0.59%) between the proportion of
phonons of the two types of MGTA is much smaller than that in
the range of 0–20 THz (1.29%). Therefore, for the cross-plane ther-
mal conduction, an increase in the number of layers results in an
increase of low-frequency phonons, especially in the range of 0–
20 THz. Therefore, a higher cross-plane thermal conductivity can
be obtained by 6-layer MGTA. It should be noted that this phe-
nomenon is different from the in-plane thermal conduction and
VDOS in x-direction.
In addition, comparison of VDOS of 6-layer MGTA with twist
angles of 10° and 30° can be seen in Fig. 14, and it can reveal the
phonon characteristics of cross-plane conduction with different
twist angles. In both intervals of 0–20 THz and 20–40THz, the pro-
portion of phonons for MGTA with the twist angle of 10° are appar-
ently higher than that of 30°. This indicates that the increase in
twist angles leads to a reduction in low-frequency phonons all
Fig. 12. Relationship between the twist angle and the cross-plane interfacial
conductance of 6-layer MGTA at different temperatures.
 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173
Fig. 13. Comparison of VDOS in z-direction of 4-layer and 6-layer MGTA without
twist angles. (a) VDOS; (b) The histogram of frequency distribution of phonons.
the time. Moreover, the roughness of the interface where the twist
angle exists can also be considered as a vital factor affecting the
cross-plane thermal conduction. If there’s no twist angle between
layers, phonons transfer between adjacent layers ballistically. Nev-
ertheless, as the interlayer twist angles increase, the structural
inconsistency between layers increases correspondingly and there
would be more scattering centers blocking the phonon transport.
4. Discussion
Both in-plane and cross-plane thermal transports of MGTA are
further discussed and the development prospect would be pro-
posed in this section:
Firstly, the size effect of the MGTA should be further evaluated.
In this study, only one specific size of the MGTA with a cross area of
22 nm
10 nm was studied, and the maximum thermal conduc-
tivity of 647.83 W/mK can be obtained with bilayer MGTA without
twist angle. This is because of the relatively small size of MGTA.
Compared to some existing studies [1,18,22,41], the maximum
thermal conductivity can reach more than 2000 W/mK, because
sizes of the simulated configurations or samples are thousands of
nanometers, and even reach a level of the micrometer in their stud-
ies. Wei et al. [23] also indicated that there’s a linear relationship
171
Fig. 14. Comparison of VDOS in z-direction of 6-layer MGTA with twist angles of
10° and 30°. (a) VDOS; (b) The histogram of frequency distribution of phonons.
between the system size and thermal conductivity. Generally, the
limited system size would cut-off the contribution of long wave-
length phonons, and a small size in the direction that is parallel
to the temperature gradient can enhance the phonon scattering.
In this study, the focus is to understand the thermal transport char-
acteristics of MGTA, and the relationship among thermal conduc-
tivity, temperatures and twist angles was proposed. Nevertheless,
the absolute value of thermal conductivity isn’t paid special atten-
tion to in this study. Whether the size of MGTA would affect the
relationship or even lead to a different conclusion would be stud-
ied in our future work.
Secondly, in this study, mechanisms behind the thermal trans-
port of MGTA are analyzed via VDOS. Although VDOS can provide
the explanation as shown in Figs. 7, 9, 13 and 14 to some extents, it
can be seen that the difference of proportions of low-frequency
phonons in each configuration ranges from about 0.5%1.0%. This
may be not enough to explain the significant difference in thermal
conductivity and interfacial conductance, and some other factors
dominate the thermal conduction. Some studies on the bilayer
MGTA [27,32] indicated that the modification of the Brillouin zone
due to the introduction of twist angles enhances the phonon scat-
tering, thus resulting in a reduction of thermal conductivity. How-
ever, to the best of the authors’ knowledge, the modification of
Brillouin zone for the MGTA, especially the effect of the position
172 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173
of twist angles are rarely reported in published literature, because
this would be a complex task. This study provides a primary inves-
tigation and a foundation to study the deep mechanism of thermal
conduction of the MGTA. The authors are devoted to revealing the
deep mechanism in future works.
5. Conclusions
In this study, the effect of interlayer twist angles of MGTA at dif-
ferent temperatures, different numbers of layers are studied com-
prehensively utilizing NEMD, and both in-plane and cross-plane
conduction are considered. Moreover, phonon characteristics
behind thermal transport are also analyzed. This study can provide
an open opportunity to study the thermal transport of the MGTA.
Some conclusions can be summarized as the following:
(1) In this study, the highest thermal conductivity can only be
obtained without interlayer twist angles no matter in-
plane and cross-plane thermal conduction. Particularly, for
in-plane thermal conduction, a slight twist angle in the
range of 0–10° could result in a sharp reduction in thermal
conductivity by about 13%.
(2) For in-plane conduction, a slight twist angle leads to a signif-
icant reduction in the thermal conductivity when the twist
angle ranges from 0° to 10°. When the twist angle changes
in the range of 10–20°, the twist angle have a slight effect
on thermal conductivity. When the twist angle increases to
30°, there’s a local maximum value. Besides, the position
where the twist angle exists also affects the thermal conduc-
tivity of the MGTA.
(3) For cross-plane conduction, the characteristics of the con-
duction is quite different from that of the in-plane conduc-
tion. In terms of MGTA without twist angles, thermal
conductivity increases as the number of layers increases. In
addition, as the interlayer twist angle increases from 0° to
30°, the interfacial thermal conductance decreases mono-
tonically with a local minimum value (rather than a local
maximum value).
Acknowledgment
The work is supported by Innovation Development and Demon-
stration Project of Ocean Economy (Grant No. BHSF2017-19),
National Natural Science Foundation of China (Grant No.
51776138) and Tianjin Talent Development Special Support Pro-
gram for High-Level Innovation and Entrepreneurship Team.
Conflict of interest
The authors declared that there is no conflict of interest.
References
[1] A.A. Balandin, Thermal properties of graphene and nanostructured carbon
materials, Nat. Mater. 10 (8) (2011) 569–581.
[2] S. Ghosh, W. Bao, D.L. Nika, S. Subrina, E.P. Pokatilov, C.N. Lau, A.A. Balandin,
Dimensional crossover of thermal transport in few-layer graphene, Nat. Mater.
9 (7) (2010) 555–558.
[3] Guanming Yuan, Xuanke Li, Zhijun Dong, Xiaoqing Xiong, Brian Rand,
Zhengwei Cui, Ye Cong, Jiang Zhang, Yanjun Li, Zhongwei Zhang, Junshan
Wang, Pitch-based ribbon-shaped carbon-fiber-reinforced one-dimensional
carbon/carbon composites with ultrahigh thermal conductivity, Carbon 68
(2014) 413–425.
[4] D.L. Nika, A.A. Balandin, Two-dimensional phonon transport in graphene, J.
Phys. Condens. Matter 24 (23) (2012).
[5] Alexander A. Balandin, Suchismita Ghosh, Wenzhong Bao, Irene Calizo,
Desalegne Teweldebrhan, Feng Miao, Chun Ning Lau, Superior thermal
conductivity of single-layer graphene, Nano Lett. 8 (3) (2008) 902–907.
[6] S. Ghosh, I. Calizo, D. Teweldebrhan, E.P. Pokatilov, D.L. Nika, A.A. Balandin, W.
Bao, F. Miao, C.N. Lau, Extremely high thermal conductivity of graphene:
prospects for thermal management applications in nanoelectronic circuits,
Appl. Phys. Lett. 92 (15) (2008).
[7] W. Cai, A.L. Moore, Y. Zhu, X. Li, S. Chen, L. Shi, R.S. Ruoff, Thermal transport in
suspended and supported monolayer graphene grown by chemical vapor
deposition, Nano Lett. 10 (5) (2010) 1645–1651.
[8] J.H. Seol, I. Jo, A.L. Moore, L. Lindsay, Z.H. Aitken, M.T. Pettes, X. Li, Z. Yao, R.
Huang, D. Broido, N. Mingo, R.S. Ruoff, L. Shi, Two-dimensional phonon
transport in supported graphene, Science 328 (5975) (2010) 213–216.
[9] Yun-Hong Zhao, Wu. Zhen-Kun, Shu-Lin Bai, Thermal resistance measurement
of 3D graphene foam/polymer composite by laser flash analysis, Int. J. Heat
Mass Transf. 101 (2016) 470–475.
[10] A.P. Kauling, A.T. Seefeldt, D.P. Pisoni, R.C. Pradeep, R. Bentini, R.V.B. Oliveira, K.
S. Novoselov, A.H. Castro Neto, The worldwide graphene flake production, Adv.
Mater. 30 (44) (2018).
[11] Peter Bøggild, The war on fake graphene, Nature 562 (2018) 502–503.
[12] L. Lindsay, D.A. Broido, Natalio Mingo, Diameter dependence of carbon
nanotube thermal conductivity and extension to the graphene limit, Phys.
Rev. B 82 (16) (2010).
[13] D.L. Nika, E.P. Pokatilov, A.S. Askerov, A.A. Balandin, Phonon thermal
conduction in graphene: role of Umklapp and edge roughness scattering,
Phys. Rev. B 79 (15) (2009).
[14] Saeed Bazrafshan, Ali Rajabpour, Thermal transport engineering in amorphous
graphene: non-equilibrium molecular dynamics study, Int. J. Heat Mass Transf.
112 (2017) 379–386.
[15] Zhiwei Ding, Qing-Xiang Pei, Jin-Wu Jiang, Wenxuan Huang, Yong-Wei Zhang,
Interfacial thermal conductance in graphene/MoS2 heterostructures, Carbon
96 (2016) 888–896.
[16] Xianhua Nie, Li Zhao, Shuai Deng, Yue Zhang, Molecular dynamic study on
crossover of equilibrium time of conduction for silicon/silicon and silicon/
silicon carbide pairs on nanoscale, Int. Commun. Heat Mass Transf. 98 (2018)
85–95.
[17] Chao Si, Xiao-Dong Wang, Zhen Fan, Zhi-Hai Feng, Bing-Yang Cao, Impacts of
potential models on calculating the thermal conductivity of graphene using
non-equilibrium molecular dynamics simulations, Int. J. Heat Mass Transf. 107
(2017) 450–460.
[18] X. Xu, L.F. Pereira, Y. Wang, J. Wu, K. Zhang, X. Zhao, S. Bae, C. Tinh Bui, R. Xie, J.
T. Thong, B.H. Hong, K.P. Loh, D. Donadio, B. Li, B. Ozyilmaz, Length-dependent
thermal conductivity in suspended single-layer graphene, Nature Commun. 5
(2014) 3689.
[19] Bing-Yang Cao, Ji-Hang Zou, Hu Guo-Jie, Gui-Xing Cao, Enhanced thermal
transport across multilayer graphene and water by interlayer
functionalization, Appl. Phys. Lett. 112 (4) (2018).
[20] Yali Ma, Zhongwei Zhang, Jige Chen, Kimmo Sääskilahti, Sebastian Volz, Jie
Chen, Ordered water layers by interfacial charge decoration leading to an
ultra-low Kapitza resistance between graphene and water, Carbon 135 (2018)
263–269.
[21] Tomasz Wejrzanowski, Mateusz Grybczuk, Mateusz Wasiluk, Krzysztof J.
Kurzydlowski, Heat transfer through metal-graphene interfaces, AIP Adv. 5 (7)
(2015).
[22] Ajing Cao, Molecular dynamics simulation study on heat transport in
monolayer graphene sheet with various geometries, J. Appl. Phys. 111 (8)
(2012).
[23] Zhiyong Wei, Zhonghua Ni, Kedong Bi, Minhua Chen, Yunfei Chen, In-plane
lattice thermal conductivities of multilayer graphene films, Carbon 49 (8)
(2011) 2653–2658.
[24] Y. Cao, V. Fatemi, A. Demir, S. Fang, S.L. Tomarken, J.Y. Luo, J.D. Sanchez-
Yamagishi, K. Watanabe, T. Taniguchi, E. Kaxiras, R.C. Ashoori, P. Jarillo-
Herrero, Correlated insulator behaviour at half-filling in magic-angle graphene
superlattices, Nature 556 (7699) (2018) 80–84.
[25] Y. Cao, V. Fatemi, S. Fang, K. Watanabe, T. Taniguchi, E. Kaxiras, P. Jarillo-
Herrero, Unconventional superconductivity in magic-angle graphene
superlattices, Nature 556 (7699) (2018) 43–50.
[26] Matthew Yankowitz, Shaowen Chen, Hryhoriy Polshyn, K. Yuxuan Zhang, T.
Taniguchi Watanabe, David Graf, Andrea F. Young, Cory R. Dean, Tuning
superconductivity in twisted bilayer graphene, Science 363 (2019) 1059–1064.
[27] H. Li, H. Ying, X. Chen, D.L. Nika, A.I. Cocemasov, W. Cai, A.A. Balandin, S. Chen,
Thermal conductivity of twisted bilayer graphene, Nanoscale 6 (22) (2014)
13402–13408.
[28] D.L. Nika, A.A. Balandin, Phonons and thermal transport in graphene and
graphene-based materials, Rep. Prog. Phys. 80 (3) (2017).
[29] Hu. Jiuning, Xiulin Ruan, Yong P. Chen, Thermal conductivity and thermal
rectification in graphene nanoribbons: a molecular dynamics study, Nano Lett.
9 (7) (2009) 2730–2735.
[30] A.I. Cocemasov, D.L. Nika, A.A. Balandin, Engineering of the thermodynamic
properties of bilayer graphene by atomic plane rotations: the role of the out-
of-plane phonons, Nanoscale 7 (30) (2015) 12851–12859.
[31] Alexandr I. Cocemasov, Denis L. Nika, Alexander A. Balandin, Phonons in
twisted bilayer graphene, Phys. Rev. B 88 (3) (2013).
[32] Chenyang Li, Bishwajit Debnath, Xiaojian Tan, Su. Shanshan, Xu. Kui, Supeng
Ge, Mahesh R. Neupane, Roger K. Lake, Commensurate lattice constant
dependent thermal conductivity of misoriented bilayer graphene, Carbon
138 (2018) 451–457.
[33] Steve Plimpton, Fast parallel algorithms for short–range molecular dynamics,
J. Comput. Phys. 117 (1995) 1–19.
 X. Nie et al. / International Journal of Heat and Mass Transfer 137 (2019) 161–173
[34] Alexander Stukowski, Visualization and analysis of atomistic simulation data
with OVITO–the open visualization tool, Modell. Simulat. Mater. Sci. Eng. 18
(1) (2010).
[35] L. Lindsay, D.A. Broido, Optimized Tersoff and Brenner empirical potential
parameters for lattice dynamics and phonon thermal transport in carbon
nanotubes and graphene, Phys. Rev. B 81 (20) (2010).
[36] L.A. Girifalco, Miroslav Hodak, Roland S. Lee, Carbon nanotubes, buckyballs,
ropes, and a universal graphitic potential, Phys. Rev. B 62 (19) (2000) 13104–
13110.
[37] J.E. Turney, A.J.H. McGaughey, C.H. Amon, Assessing the applicability of
quantum corrections to classical thermal conductivity predictions, Phys. Rev. B
79 (22) (2009).
173
[38] Jennifer R. Lukes, Hongliang Zhong, Thermal conductivity of individual single-
wall carbon nanotubes, J. Heat Transf. 129 (2007) 705–716.
[39] L. Cui, Y. Feng, P. Tan, X. Zhang, Heat conduction in double-walled carbon
nanotubes with intertube additional carbon atoms, PCCP 17 (25) (2015)
16476–16482.
[40] Zhiyong Wei, Zhonghua Ni, Kedong Bi, Minhua Chen, Yunfei Chen, Interfacial
thermal resistance in multilayer graphene structures, Phys. Lett. A 375 (8)
(2011) 1195–1199.
[41] A. Bagri, S.P. Kim, R.S. Ruoff, V.B. Shenoy, Thermal transport across twin grain
boundaries in polycrystalline graphene from nonequilibrium molecular
dynamics simulations, Nano Lett. 11 (9) (2011) 3917–3921.