Journal of Non-Crystalline Solids 546 (2020) 120284

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Journal of Non-Crystalline Solids

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

Strengthening and toughening mechanisms of metallic glass nanocomposites T

via graphene nanoplatelets
⁎,b
Zhuocheng Xiea,c, Wu-Rong Jian , Xiaochang Tanga, Xiaoqing Zhanga, Xiaohu Yaoa,c
a
Department of Engineering Mechanics, South China University of Technology, Guangzhou, Guangdong 510640, P. R. China
b
Department of Mechanical Engineering, University of California, Santa Barbara, Santa Barbara, California 93106, USA
c
State Key Laboratory of Subtropical Building Science, South China University of Technology, Guangzhou, Guangdong 510640, PR China

A R T I C LE I N FO A B S T R A C T

Keywords: The lack of ductility, mainly due to shear localization, limits the full exploitation of metallic glasses (MGs). Such
Strengthening and toughening a weakness can be mitigated via introducing graphene nanoplatelets (GNs), which helps strengthen and toughen
Metallic glass nanocomposites MG matrix. Using molecular dynamics simulations, we investigate the tensile deformation of Cu50Zr50 metallic
Graphene nanoplatelets glass-graphene nanoplatelet composites (MGGNCs) regarding the effects of graphene volume fraction and gra-
Molecular dynamics simulations
phene layer number. Increasing fraction of GN in MGGNC enhances both tensile strength and fracture strain. The
dominant component changes from MG matrix to GN, corresponding to a failure mode transition from shear
banding in MG to brittle fracture in graphene. For a given volume fraction, single-layered GN behaves better
than its double-layered counterpart, manifested as a higher fracture strain in MGGNCs. Our study illustrates the
strengthening and toughening mechanisms in MGGNCs, and why single-layered GN performs better. All of these
results can contribute to the synthesis of novel MG/graphene composites.

1. Introduction crystalline nanolaminates and introduced grain boundaries or glass-

Metallic glasses (MGs) have attracted great research interests over
the past decades for superior strength and high elastic limit, but they
generally lack tensile ductility that results in sudden and catastrophic
failure [1–4]. It is found that the rapid propagation of shear bands (SBs)
formed by localizing shear transformation zones (STZs), is the chief
culprit in most abrupt failures of MGs, especially under tensile loading
[5–7]. Therefore, solutions are investigated to avoid shear banding of
MGs and attain high ductility. Through all approaches to large ductility,
one is reducing the external dimensions of MGs to the order of 100 nm
[8–10], and the other common access is developing heterogeneity in
MGs by the adoption of the second phase. For example, introducing
amorphous-crystalline interfaces can effectively impede the propaga-
tion of SBs in MGs, leading to a more homogeneous strain distribution
and thus better ductility [11,12]. Hofmann et al. claimed that utilizing
the inhomogeneous microstructure with isolated dendrites in a MG
matrix could stabilize the glass against the catastrophic failure asso-
ciated with unlimited extension of a shear band and result in enhanced
global plasticity [13]. Besides, Zhou et al. [14] took advantage of
amorphous-amorphous interfaces and soft amorphous component to
constrain SB propagation in MGs, which also enhanced ductility.
Moreover, Jian et al. [15,16] tuned the layer thickness of amorphous-
glass interfaces into the laminates or the bulk MGs, which boosted the
plasticity of the MG matrix, hence balancing the trade-off between
ductility and strength as well as hardness.
Meanwhile, graphene was invented as an excellent material with
high intrinsic strength and Young’s modulus [17–20], and three-di-
mensional graphene-reinforced metallic composites have become in-
creasingly interesting in recent years [21–24]. Kim et al. [25] conduted
nanopillar compression experiment and molecular dynamics simula-
tions to Cu (or Ni)-graphene nanolayered composites and reported that
dislocations were unable to penatrate graphene-metal interface, leading
to high strength of composites. Similar compression experiment for
graphene-Al nanolaminates indicated that graphene strengthened and
toughened the metal matrix as a result of the enhanced interface-dis-
location interactions and crack deflection by the robust graphene-Al
interfaces in the composites [26–28]. Hwang et al. [29] found that
graphene blocked fatigue cracks generated during cyclic bending tests
in Cu-graphene nanolayered composites, which greatly improved their
ductility. Liu et al. [30–32] systematically studied Cu-graphene nano-
layered composites under shear loading and the results showed that
graphene could amplify anti-fatigue properties by hindering disloca-
tions propagation.
Since graphene has been thought to be an ideal reinforcement

⁎
Corresponding author.
E-mail addresses: wurong@ucsb.edu (W.-R. Jian), tcqzhang@scut.edu.cn (X. Zhang).

https://doi.org/10.1016/j.jnoncrysol.2020.120284
Received 13 May 2020; Received in revised form 1 July 2020; Accepted 2 July 2020
0022-3093/ © 2020 Elsevier B.V. All rights reserved.
Z. Xie, et al.
material, the combination of MGs and graphene for enhanced strength
and ductility is taken into account. Park et al. [33] reported experi-
mental evidence that MG-graphene nanolaminate exhibited high elastic
modulus and yield strength. Homogeneous flow improving tensile
ductility of nanolaminates was realized through tailoring the thickness
of MG layers. To the best of our knowledge, previous studies of gra-
phene-reinforced nanocomposites mostly focus on their mechanical
properties and the reinforcement effects of either single - layered gra-
phene [34–37] or different distributions of single - layered graphene
[38], neglecting the interaction between different layers of graphene
due to the existence of interface [39,40] and their behavior during
deformation, which should be compared with their single - layered
counterpart when chosing the ideal reinforcement. Moreover, while
some computational work have been conducted to study the mechan-
ical behaviors of carbon nanotube (or Cu nanowire)-MG nanocompo-
sites [41,42], simulation investigations at atomistic scale about MG-
graphene nanocomposites have been rarely reported [38,43]. Since it is
generally difficult to fully capture microscopic phenomena in-situ ex-
periments, molecular dynamics (MD) simulations serve as a powerful
tool to explain atomistic mechanisms at nano scale [16,44].
In the present work, we perform MD simulations to study the tensile
behaviors of metallic glass-graphene nanoplatelet composites
(MGGNCs) with different graphene volume fractions and graphene
layer numbers. As shown by previous studies about metallic glass
consisting of different composites, CuZr MG has been widely in-
vestigated with relatively outstanding properties such as high elastic
modulus and ultimate strength [41,42]. Thus we select Cu50Zr50 MG as
a representative for further investigation. For MGs reinforced by
single - layered graphene nanoplatelets (SLGNs), increasing graphene
volume fraction significantly improves ultimate tensile strength and
toughness of MGGNCs, and plastic deformation mode transits from
shear localization to homogeneous flow as graphene volume fraction
rises. Moreover, less ductility is observed in composites with double -
layered graphene nanoplatelets (DLGNs) than those with SLGN at the
approximate graphene volume fraction. The subsequent analysis re-
veals the poor behavior of MGGNCs with DLGN is ascribed to the in-
compatible deformation between two graphene layers.
The paper is organized as follows. Details of atomistic simulations
including modeling, loading and analysis methods, are presented in
Section 2. In Section 3, strengthening and toughening mechanisms as
well as failure modes of MGGNCs are discussed. The paper is concluded
in Section 4.
2. Methodology
2.1. Models and computations
A small Cu50Zr50 MG model, composed of 10,000 atoms, is built by
melting the initial alloy configuration at 2000 K and then cooling it to
50 K at the rate of 0.01 K/ps. During this process, constant-pressure-
temperature (NPT) ensemble and three-dimensional periodic boundary
conditions are applied. The detailed procedures to produce the small
MG cube can be found in Ref. [45]. To construct the final Cu50Zr50 MG
matrix, the small MG cube is replicated to reach a large sample with
required dimensions. In addition to one pure MG, eight different con-
figurations of MGGNCs are taken into account in this study and their
schematics are shown in Fig. 1. As Fig. 1 (a) shows, dimensions of all
configurations along x-, y-, z- directions are ~ 58 nm × 29 nm ×
5.8 nm, respectively. Sample I is pure MG, II to VII are metallic glass-
single - layered graphene nanoplatelet composites (MGSLGNCs) with
different graphene volume fractions (The length of graphene along x-
axis is the same as that of MG). Sample VIII and IX are metallic glass-
double - layered graphene nanoplatelet composites (MGDLGNCs).
Given a certain graphene volume fractions, V and VIII (or VI and IX) are
the control group, in which graphene layer number is the variable. The
layer number and volume fraction of graphene of all configurations are
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Journal of Non-Crystalline Solids 546 (2020) 120284
listed in Table 1. For MGDLGNCs, distance between two graphene layer
is 3.4 Å [46]. The chirality of graphene in all samples along x axis is
zigzag.
Boundary conditions of all samples along three dimensions are set to
be periodic during equilibration under isothermal-isobaric (NPT) en-
semble with a constant temperature at 50 K and zero pressure. Here the
low temperature (50 K) is used to highlight the material responses upon
mechanical activation, since the simulated glass structure constructed
with high quenching rate is usually more prone to thermal activation
than MGs used in experiments, which have much longer time to relax
[47]. After relaxation, uniaxial tension along the x axis at a constant
strain rate of 1 × 108 s−1 is imposed to all samples, during which
boundary conditions along x and z axes are remained periodic (zero
pressure along z direction) while that along y axis is adjusted to shrink -
wrapped. Timestep in all MD simulations is 2 fs. Such a timestep is
widely used in MG uniaxial simulations at the strain rate of ~ 109 s−1,
which have been proved to be capable of fully capturing the accumu-
lation of STZs and the formation of SBs [48,49]. Moreover, a strain
increment of about 5 ∼ 10 × 10−7 (corresponding to a timestep of
0.5 ~ 1 fs at the strain rate of 109 s−1) provides enough accuracy for
describing the deformation and fracture processes of graphene under
uniaxial loading [50,51]. Here, the step length of tensile strain is
2 × 10−7, which is believed to be accurate enough for reflecting the
deformation details and illustrating the deformation mechanisms of
MGGNCs. Simulations are performed using the Large - scale Atomic/
Molecular Massively Parallel Simulator (LAMMPS) [52] and the cor-
responding results are visualized by the Open Visualization Tool
(OVITO) [53].
2.2. Interatomic potentials
Since atomic interactions for MGGNCs include: (1) the interactions
between metallic atoms in the MG matrix, (2) the interactions between
carbon atoms in GN, and (3) the interactions between carbon atoms and
metallic atoms, different potentials are considered to describe the in-
teractions above. In this study, embedded atom method (EAM) poten-
tial developed by Mendelev et al. [54] is used to simulate metallic
atomic interactions. Additionally, AIREBO potential [20] is adopted to
define interactions among carbon atoms. Van der Waals forces between
GN and MG matrix is described by Lennard-Jones potential, which has
been widely utilized to convey non-bonded interactions, as shown in
Eq. 1:
σ σ
ELJ = 4ϵ[ ⎛ ⎞ 12 − ⎛ ⎞ 6],
⎝r ⎠ ⎝r ⎠ (1)
where σ is the interatomic separation when the value of potential is zero
and ϵ is the depth of the potential well. The related parameters are
listed in Table 2, which are calculated according to methods proposed
by Reza Rezaei using Lorentz–Berthelot mixing rule [55]. For Cu,
σCu − Cu = 2.29726, ϵCu − Cu = 0.52031 were used as in Ref [56]. For Zr,
σZr − Zr = 2.9318, ϵZr − Zr = 0.73847 were adopted following Ref [57]. For
the non-bonded C atoms, σC − C = 3.4, ϵC − C = 0.00284 were taken from
Ref [20]. σC-Cu and σC-Zr are obtained via σ12 = (σ11 + σ22)/2 while ϵC-Cu
and ϵC-Zr are calculated by ϵ12 = ϵ11ϵ22 . This fitting method and values
for LJ parameters of non - equal atoms have been validated by previous
studies to depict the interfacial potentials between C-Cu and C-Zr
[38,43,55]. The cutoff distance for Lennard - Jones potential is set as
rc = 8.06 Å. The total potential energy for MGGNCs is calculated as
Eq. 2:
C − Cu C − Zr
Etotal = EEAM + EAIREBO + ELJ + ELJ . (2)
Z. Xie, et al. Journal of Non-Crystalline Solids 546 (2020) 120284

Fig. 1. (a) Three-dimensional sizes of each sample. Atomic configurations with different graphene volume fractions: (b) 0%, (c) 0.17%, (d) 0.52%, (e) 1.03%, (f)
1.63%, (g) 3.27%, (h) 5.76%, (i) 1.72%, (j) 3.27%. (b) denotes pure MG. The configurations in (c)–(h) and (i)–(j) have single-layered graphene nanoplatelets and
double-layered graphene nanoplatelets inserted, respectively.

Table 1 whole sample, corresponding to the sharp drop after peak stress in
The layer number (n) and graphene volume fraction (vGr%) in all samples stress-strain curve. In contrast, increasing graphene volume fraction in
(pure MG or MGGNCs). MGSLGNCs can significantly improve the ultimate tensile strength and
Sample n vGr% toughness of composites. When graphene volume fraction is at or under
1.63%, all curves of MGSLGNCs exhibit three stages. Here, we take
I ––– ––– sample II as an example (Fig. 3 (a)). Stage A represents the elastic
II one 0.17%
period and initial plastic stage, during which the stress continues to
III one 0.52%
IV one 1.03% rise. In stage B, notable plastic deformation occurs and the stress de-
V one 1.63% clines upon reaching the ultimate tensile strength, which corresponds to
VI one 3.27% the formation of a single, dominant shear band. In stage C, stress
VII one 5.76% fluctuates with the increase of strain, as SB continues to grow and the
VIII two 1.72%
IX two 3.27%
sample starts sliding along the SB. Finally, there is a rapid drop of stress.
Such a stress decrease indicates graphene has fractured and the sample
fails. As shown in last inset of Fig. 3 (a), SLGN is rolled seriously in the
Table 2 region where SB traverses the sample, leading to the fracture of SLGN.
The parameters of LJ potential for different types of atomic interactions. For MGSLGNCs with graphene volume fractions of 3.27% and 5.76%
(sample VI and VII), their tensile stresses increase continuously to the
Atomic interaction σ\Å ϵ\eV
maximum value, where the fracture of graphene begins. For example,
C-Cu 2.84863 0.03844 the stress-strain curve of sample VI is displayed in Fig. 3 (b). Without a
C-Zr 3.1659 0.0458 dominant SB in this situation, SLGN seems to be ripped directly for
overloading, resulting in the sudden failure of the sample. By com-
paring Fig. 3 (a) and (b), there exists a transition of dominant de-
3. Results and discussion formation mechanism from shear banding in MG matrix to brittle
fracture in graphene.
3.1. MGSLGNCs

3.1.1. The tensile behaviors of MGSLGNCs 3.1.2. Shear banding in MGSLGNCs

Fig. 2 depicts the tensile engineering stress - strain curves for pure
MG and MGSLGNCs with graphene volume fractions ranging from
0.17% to 5.76%. Pure MG expires when SBs propagate through the
Fig. 2. Tensile stress - strain curves of pure MG and MGSLGNCs with different
graphene volume fractions.
To further understand shear banding in MGSLGNCs and the tran-
sition of the deformation mechanism, atomic shear strain analysis [58]
is performed. Since the regions with large atomic shear strain also bear
severe localized plastic deformation, we only remain MG atoms with
atomic shear strain above 0.4, corresponding to the STZ clusters. For
samples with graphene volume fraction not exceeding 1.63% (sample I-
5), Fig. 4 shows snapshots of STZs and SLGNs during tensile loading. As
shown in Fig. 4 (a), STZs are triggered at the free surface of pure MG
sample and increase with further loading. After STZs converging into a
single SB, its propagation across the sample results in the subsequent
failure. Slightly different from those in pure MG, STZs in MGSLGNCs
are also generated at MG-SLGN interfaces where stress concentration
prevails (See the insert of Fig. 4 (d)). With higher graphene volume
fractions, the initiation of STZs is delayed by more pronounced re-
inforcement effects of graphene, characterized by later moment that
STZs appear (See the first columns of Fig. 4 (a)–(e)). Thus, the propa-
gation of SB is also postponed. Meanwhile, SLGNs remain undamaged
and stay in a mild atomic strain level during the activation and growth
of STZs. Therefore, the promotion in the tensile strength of MGSLGNCs
results from the load sharing of SLGN and the improvement of tough-
ness in MGSLGNCs is due to the obstruction to single dominant SB
generation and the succedent load-bearing capacity of SLGN after the
formation of SB.
To verify the influence of graphene volume fraction on the sup-
pression to SB, the thickness of SB is measured after removing MG

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Z. Xie, et al. Journal of Non-Crystalline Solids 546 (2020) 120284

Fig. 3. Schematic illustrations of two representative types of stress-strain curves for MGSLGNCs with different graphene volume fractions, namely (a) sample II,
three-stage form and (b) sample VI, strain hardening form. The atoms in the insets are colored by atom shear strain.

atoms with atomic strain value under 0.4. Fig. 5 illustrates the evolu- These results confirm the transition of two governing deformation
tion of a single dominant SB during tensile loading, the profile of which mechanisms. Preeminent reinforcement effects of SLGN resist the for-
is outlined with dash lines. As illustrated in Fig. 5 (a), we denote the mation of a single dominant SB and multiple small STZs diffuse the
thickness of SBs as ‘T’ and it is estimated from the arithmetic average, strain distribution. Thus, plastic deformation pattern transits from shear
T
i.e., T = max
+
Tmin 2, where ‘Tmax ’ and ‘Tmin ’ represent the widest and the localization to homogeneous deformation. It is worth mentioning that
most narrow width of SB, respectively. As summarized in Fig. 6, the graphene controls the fracture strain of all MGSLGNCs, illustrating that
thickness of the dominant SB decreases with graphene volume fraction graphene volume fraction determines the toughness of MGSLGNCs.
increasing. Especially, for sample V, SLGN brings remarkable effect on With the increasing graphene volume fraction, tensile strength and
the suppression to the dominant SB. Obviously, the domination of the fracture strain of MG composite can be enhanced significantly
single SB vanishes with the increase in graphene volume fraction. By (Table 3).
contrast, the sample with graphene volume fraction above 1.63% (e.g.,
sample VI in Fig. 7), STZs distribute uniformly in the whole sample,
making the entire sample deform in a homogenous way. Hence, the
dominant SB is absent.

Fig. 4. The evolution from STZs to a single SB in (a) pure MG and (b)–(e) MGSLGNCs with different graphene volume fractions. Only MG atoms with atomic shear
strain above 0.4 and graphene atoms are shown. The former are all gray and the latter are colored by atomic shear strain.

4
Z. Xie, et al. Journal of Non-Crystalline Solids 546 (2020) 120284

Fig. 5. The evolution of a single SB in (a)

pure MG and (b)–(e) MGSLGNCs with dif-
ferent graphene volume fractions. The pro-
files of SBs are hinted by dash lines and
their thicknesses are denoted as ’T’. Only
MG atoms with atomic shear strain above
0.4 are shown in purple. (For interpretation
of the references to colour in this figure le-
gend, the reader is referred to the web ver-
sion of this article.)

Table 3
Tensile behaviors of pure MG and MGSLGNCs with different graphene volume
fractions (vGr%).
Sample vGr% Tensile strength\GPa Fracture strain\%

I ––– 3.90 11.4

II 0.17% 3.94 14.04
III 0.52% 4.14 17.25
IV 1.03% 4.53 17.31
VI 3.27% 6.83 20.73
VII 5.76% 9.90 21.12

3.2. MGDLGNCs

3.2.1. The tensile behaviors of MGDLGNCs

Fig. 6. The thicknesses of SBs in pure MG and MGSLGNCs with different gra-
phene volume fractions.
Fig. 7. The evolution of STZs in sample VI. Only MG atoms with atomic shear
strain above 0.4 and graphene atoms are shown. The former are all gray and the
latter are colored by atomic shear strain.
After considering the effect of graphene volume fraction on the
strength and ductility of MGSLGNCs, we take into account the role of
graphene layer number in deformation behaviors. Herein, MGDLGNCs,
with graphene volume fractions of 1.72% and 3.27% (sample VIII in
Fig. 1 (i) and IX in Fig. 1 (j)), are compared to their MGSLGNC coun-
terparts with the approximating graphene volume fractions (1.63% for
sample V and 3.27% for sample VI), respectively. From the stress -
strain curves in Fig. 8 (a), it is seen that each pair of curves with similar
graphene volume fraction coincide with each other before stress drop or
further enhancement in plastic deformation, emphasizing that the
elastic and initial plastic regime prominently depends on graphene
volume fraction. This is because MG is sufficient to withstand external
loads and the number of GN rarely affects deformation behaviors
during these periods. Nevertheless, once plastic deformation proceeds,
the curves of MGDLGNCs fall below their MGSLGNC counterparts. This
suggests smaller single-layered graphene surface area in MGDLGNCs
gives rise to a limited enhancement in comparison to the corresponding
cases of MGSLGNCs at given graphene volume fraction. Consequently,
SLGN imposes more considerable strengthening effect than DLGN at a
given graphene volume fraction. Akin to Fig. 3 (a) and (b), the curves in
Fig. 8 (b) and (c) also show three-stages mode and strain-hardening
mode, respectively. Such phenomena reveal that the transition in
plastic deformation mode mentioned above also exists in MGDLGNCs.

5
Z. Xie, et al.
Fig. 8. (a) Tensile Stress - strain curves of MGSLGNCs and MGDLGNCs (plotted in dash lines) with the approximating graphene volume fractions. Schematic
illustrations of two representative types of curves for MGDLGNCs with different graphene volume fractions, namely (b) sample VIII, three-stage form and (c) sample
IX, strain hardening form.
Interestingly, although graphene has an important impact on the frac-
ture strain of all MG - GN composites, MGDLGNC shows a worse duc-
tility than MGSLGNC at similar graphene volume fraction. What we
observe indicates that the ductility of MG-GN composites is affected by
both graphene volume fraction and the number of GNs.
3.2.2. The interfaces of GN-GN and MG-GN
To explain the unsatisfactory ductility of MGDLGNCs, we pay at-
tention to GN-GN and MG-GN interfaces (Fig. 9). Here, only GN layer
and the neighboring MG layers with the thickness of 2 Å are shown. At
first, we divide the whole x − y plane into numerous bins by binning
analysis and calculate the average coordinate along z axis for atoms in
each bin in all the GN and MG layers, respectively. Then, the distances
of different interface are defined as the differences of these average
coordinates we calculate. Finally, a contour for the distance between
various interfaces are obtained. Fig. 10 (a)–(c) depict the distance dis-
tributions of three interfaces, i.e., upper GN-lower GN interface, upper
MG-upper GN interface and lower GN-lower MG interface, in sample
VIII at the tensile strain of 15.48%. As seen from Fig. 10 (a), the two
ends of DLGN show much larger interface distance than its remaining
area, pointed by dash lines. In comparison to GN-GN interface, the
distance distribution between MG-GN interface exhibit a com-
plementary result (Fig. 10 (b) and (c)). Since GN-GN and MG-GN in-
terfaces are constrained by Van der Waals force and the original dis-
tance between DLGN is about 3.4 Å, much less than the maximum
distance values after intense deformation, interface debonding may
arise.
To better understand such a distribution of interface distance be-
tween DLGN, its three-dimensional schematic illustration and the dis-
tributions of atomic shear strain in MG matrix and GNs as well as the
distorted shape of DLGN are presented in Fig. 10 (d)–(f). According to
the distance value shown in Fig. 10 (d), local regions with larger value
have distinct orientations, in accordance with the directions of the
dominant SBs lying at two ends of the sample, where GNs seriously
deform (See arrows EF and GH in Fig. 10 (d) and arrows E ′F ′ and G ′H ′
in Fig. 10 (e)). This reveals that the generation of the dominant SB and
Fig. 9. Schematic illustration of the measurement of distances between dif-
ferent interfaces in MGDLGNC. Only GN layer and the neighboring MG layers
with the thickness of 2 Å are shown.
6
Journal of Non-Crystalline Solids 546 (2020) 120284
its movement have significant effect on the warp of DLGN, which leads
to the deformation incompatibility in different neighboring regions of
DLGN (Fig. 10 (a)). As a result, DLGN prones to fracture.
In addition, the similar computation involving interface distances is
applied to sample IX. The calculation results of upper GN-lower GN
interface, upper MG-upper GN interface and lower GN-lower MG in-
terface at the tensile strain of 16.07% are illustrated in Fig. 11 (a)–(c),
respectively. Unlike the deformation mode of the previous MG - DLGN
sample mentioned above, the interface distance distribution shown in
Fig. 11 are much more homogeneous in most areas, which results from
the absence of the dominant SB in plastic regime (See inserts of Fig. 8
(c)). However, the deformation incompatibility of DLGN still appears
during tension in plastic stage (denoted by dash line in Fig. 11 (a)). As a
result, crack in the GNs initiates at the boundary of the incompatible
area (See Fig. 11 (d)), which is in line with the fracture mode of the
preceding MGDLGNC and gives rise to poor ductility compared with its
MGSLGNC counterpart with similar graphene volume fraction. Based
on the above-mentioned analysis, MGSLGNCs show more promising
performance than MGDLGNCs. Moreover, the deformation incompat-
ibility of DLGN is also demonstrated as interface instability or fluc-
tuation in previous studies [32,59]. However, its fracture mechanism
that the damaged sites of DLGN lie at the boundary of the incompatible
area of interface distance, is first proposed and linked with the de-
formation incompatibility. These results provide a valuable insight to
the design of GN-reinforced composites.
4. Conclusions
In summary, we explore the strengthening and toughening effects of
SLGN and DLGN with different graphene volume fractions on the uni-
axial tensile behavior of MGGNC via MD simulations. The main con-
clusions are:
• Significant dependence of tensile strength and ductility on graphene
volume fraction are found. With an increasing fraction of single-
layered GN in metallic glass composites, both tensile strength and
fracture strain are enhanced.
• Rising graphene volume fraction effectively suppresses the forma-
tion of single dominant SB and multiple STZs prevail during the
plastic regime, which leads to a transition in the plastic deformation
mode of MGGNCs. Once the single dominant SB is impeded by GN,
plastic deformation mode transits from shear banding to homo-
geneous flow.
• Based on the comparison between MGSLGNCs and MGDLGNCs with
the similar graphene volume fraction, less ductility, due to the
earlier fracture of GN, appears in MGDLGNCs, which is rationalized
by the incompatibility of DLGN deformation. Thus, single-layered
graphene nanoplatelet behaves better than its double-layered
counterpart at a given volume fraction.
Z. Xie, et al. Journal of Non-Crystalline Solids 546 (2020) 120284

Fig. 10. Snapshots of sample VIII at the tensile strain of 15.48%. The distance distribution of (a) upper GN-lower GN interface (dash lines imply the boundary
between regions with large value and small value), (b) upper MG-upper GN interface and (c) lower GN-lower MG interface. (d) Three - dimensional view of (a).
Arrows in (d) highlight the regions with large interfacial distance. (e) The distribution of atomic strain in MG matrix and the related configuration of DLGN.
Corresponding to those in (d), arrows in (e) show the orientations of SBs. (f) The distribution of atomic strain in DLGN, where dash lines show the boundary between
regions with large value and small value, corresponding to those in (a).

Our results provide an understanding about the strengthening and
toughening mechanisms of GN-reinforced MG nanocomposites at
the nanoscale and offer a promising guideline for strong, ductile MG
composites.
CRediT authorship contribution statement
Zhuocheng Xie: Conceptualization, Methodology, Software,
Writing - original draft. Wu-Rong Jian: Data curation, Formal analysis,
Writing - review & editing. Xiaochang Tang: Formal analysis, Writing -
review & editing. Xiaoqing Zhang: Supervision, Writing - review &
editing. Xiaohu Yao: Supervision, Writing - review & editing.
Declaration of Competing Interest
The authors whose names are listed immediately below certify that
they have NO affiliations with or involvement in any organization or
entity with any financial interest (such as honoraria; educational
grants; participation in speakers’ bureaus; membership, employment,
consultancies, stock ownership, or other equity interest; and expert
testimony or patent-licensing arrangements), or non-financial interest
(such as personal or professional relationships, affiliations, knowledge
or beliefs) in the subject matter or materials discussed in this manu-
script.
Acknowledgments

The Acknowledgements session needs to be revised as: X. Yao would

7
Z. Xie, et al.
Fig. 11. Snapshots of sample IX at the tensile strain of 16.07%. The distance distribution of (a) upper GN-lower GN interface (dash lines imply the boundary between
regions with large value and small value), (b) upper MG-upper GN interface and (c) lower GN-lower MG interface. (d) The distribution of atomic strain in DLGN,
where the dash line shows the boundary between regions with large value and small value, corresponding to that in (a).
like to express his sincere gratitude for the financial support by National
Science Foundation for Distinguished Young Scholars of China
(11925203) and Natural Science Foundation of China (11672110).
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