Applied Surface Science 282 (2013) 450–455

Contents lists available at SciVerse ScienceDirect

Applied Surface Science

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

Molecular dynamics study on the equal biaxial tension of Cu/Ag

bilayer films
Lin Yuan, Zhenhai Xu, Debin Shan ∗ , Bin Guo
School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001, China

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

Article history: The mechanical behavior, dislocation nucleation and development, and the evolution of interface in
Received 27 April 2013 Cu/Ag bilayer films during an equal biaxial tension were studied using molecular dynamics simulations.
Received in revised form 29 May 2013 The results show that dislocations are prone to nucleate at the interface of Cu/Ag bilayer film, and then
Accepted 29 May 2013
propagate toward the free surface. The deformation defects consist of partial dislocations and intrinsic
Available online 4 June 2013
stacking faults, accompanying with some extrinsic stacking faults and stacking fault tetrahedra which
just occur at the interface and propagate in the Cu layer. Compared with Cu and Ag films, Cu/Ag bilayer
Keywords:
films have the maximal yield strain. The surface roughness reaches maximum at the yield strain, and
Cu/Ag bilayer films
Equal biaxial tension
then rapidly decreases with the increase of strain. Atoms in stacking faults increase with the strain at the
Interface high strain rate, while the rule is reversed at the low strain rate.
Dislocation © 2013 Elsevier B.V. All rights reserved.
Molecular dynamics

1. Introduction
Thin films have been widely used in various fields. The mechan-
ical properties of thin films are important factors constraining their
application range and service life. They cannot be directly deduced
from the mechanical properties of the corresponding bulk mate-
rials, since the thin films mechanical behavior is changed by the
dimensions substantial decrease of both the external shape and
the internal microstructure of thin films at the same time. Some
progress has been made to test the properties of thin films in experi-
mental equipments and methods on nano-scale and even on atomic
scale, but it is still very limited [1,2]. Molecular dynamics (MD)
simulations can be used to observe some unique phenomenon and
processes which cannot do in experiments, and reveal their essence
on atomic scale. In general, MD simulations can remedy the weak-
ness of experiments very well in scientific research [3–9].
Currently, most MD simulations studies on the mechanical
behavior of films were performed under the loading condition of
nanoindentation and uniaxial tension [10–14]. However, materi-
als often suffer a complex stress state in engineering applications,
so it is also necessary to study the tensile properties of films under
biaxial or multi-axial loading. Kolluri et al. [15] simulated the defor-
mation process of the single crystal Cu(1 1 1) film at a broad range
of equal biaxial tensile strains. The results show five regimes in
∗ Corresponding author at: P.O. Box 435, No. 92 West Dazhi Street, Harbin 150001,
China. Tel.: +86 451 86418732; fax: +86 451 86418732.
E-mail address: d.b.shan@gmail.com (D. Shan).
the thin film’s mechanical response with increasing strain. He et al.
[16] studied the plastic deformation behavior of the single crys-
tal Cu(0 0 1) film subjected to equal biaxial tensile strain. Although
some research has been performed on the mechanical behavior of
homogeneous films, little focus was put on films with more com-
plex structures.
Since Cu and Ag have a large lattice mismatch at the interface,
the Cu–Ag system is often regarded as a typical research object with
a large interfacial strain. A lot of attention has been attracted to the
interface structure of the Cu/Ag bilayer film [17,18]. It is well known
that defects play an important role on the properties of materi-
als, but there is little research on the deformation behavior of the
Cu/Ag bilayer film. In this paper, the equal biaxial tensile process of
the Cu/Ag bilayer film was simulated by the MD method, and was
compared with that of the single crystal Cu film and Ag film. The
deformation mechanism of different systems was investigated by
analyzing defects evolution in films.
2. Simulation methods
The atomic interaction in the Cu–Ag system was described by
the EAM potentials [19,20]. The MD tensile model of the Cu/Ag
bilayer film is shown in Fig. 1, where the x-, y- and z-axis corre-
spond to [1 1 2̄], [1̄ 1 0] and [1 1 1] of crystal, respectively. The
atoms of Cu and Ag are colored blue and red. The dimensions of
the top Cu film are 36aCu × 63aCu × 8aCu , where aCu denotes the
lattice constant of Cu, while the dimensions of the bottom Ag film
are 32aAg × 56aAg × 8aAg , resulting in a Moiré pattern structure of
the interface [18]. The free boundary condition was applied along

0169-4332/$ – see front matter © 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.apsusc.2013.05.150
 L. Yuan et al. / Applied Surface Science 282 (2013) 450–455
Fig. 1. MD tensile model of the Cu/Ag bilayer film.
z-axis, while the periodic boundary condition was applied along
the other axes. Initially, the film was relaxed with no strain for
5 ps, and then it was strained biaxially along the x and y direc-
tion up to the chosen strain level at a specific rate. Finally, the
film was relaxed for another 50 ps. The simulation parameters
are summarized in Table 1. The velocity rescaling method was
adopted to control the film at a constant temperature of 300 K.
All simulations were performed using the open codes LAMMPS
[21].
To analyze the response of the film to the applied equal biax-
ial strain, the angle distribution function (ADF) [22] method was
employed to categorize the atoms into locally perfect FCC and HCP
ones, and then identify various crystal defects based on the distri-
bution of atoms in different lattice arrangements in the film. Two
neighboring planes of HCP atoms constitute an intrinsic fault in a
FCC lattice, while two planes of HCP atoms separated by a plane of
FCC atoms constitute an extrinsic fault.
3. Results and discussion
The deformation of the Cu/Ag bilayer film is found to be elas-
tic up to a biaxial strain ε of 7.3%, beyond which the strain in
the film is relaxed by plastic deformation. It is indicated that the
value of 7.3% is the yield strain. The nucleation and propagation of
dislocations during the tensile process of the Cu/Ag bilayer film
is shown in Fig. 2, where only the atoms in stacking faults are
visible using ADF method. The two horizontal neighboring layers
of atoms appear as the Cu/Ag bilayer interface, above and below
which are Ag and Cu films, respectively. Fig. 2(a) shows that the
dislocation nucleates firstly in the Cu film from the Cu/Ag interface
at ε = 7.3%, due to the lattice misfit of the interface and the lower
stacking fault energy of Cu. Fig. 2(b) shows that when the strain ε
Table 1
Simulation parameters of the tension.
Model lx × ly × lz
36[1 1 2̄] × 63[1̄ 1 0] × 8[1 1
Cu/Ag bilayer
32[1 1 2̄] × 56[1̄ 1 0] × 8[1 1
Cu film 64[1 1 2̄] × 112[1̄ 1 0] × 16[1
Ag film 64[1 1 2̄] × 112[1̄ 1 0] × 16[1
451
reaches 8%, dislocations still nucleate firstly in the Cu film from the
interface, but the nucleation distributes more uniformly. With the
further relaxation of strain, the dislocations nucleate in the inte-
rior and free surface at the same time, and also nucleate in the Ag
film. It indicates that the dislocations prone to nucleate in the Cu
film.
Fig. 3 shows the deformation defects in the Cu/Ag bilayer film
after relaxation at ε = 7.5%. Atoms in the FCC and HCP structures are
colored green and orange in Fig. 3(a), while only those in the HCP
structure are visible in Fig. 3(b). The defects include the intrinsic
stacking faults (SFs), extrinsic SFs and SF tetrahedra, and of which
the former is the main defect type. These defects result from the
interaction between Shockley partial dislocations in different slip
planes. It is worth mentioning that stacking fault tetrahedra are
observed in a variety of strain levels, but such defects exist only in
the Cu film. The bottom surface of the stacking fault tetrahedron
consists of the first Cu atom layer at the interface, while the other
three faces extend toward the Cu film.
The surface morphologies of the Cu/Ag bilayer films subjected
to equal biaxial strains with ε = 7.3% and 10% are shown in Fig. 4,
where atoms are colored according to their relative height along
z direction. It can be observed that the surface exhibits a trian-
gle net structure, resulting from the cross of surface steps left by
dislocation movement. As the strain increases, the plastic deforma-
tion becomes more uniform, i.e., more dislocations nucleates and
uniformly distribute in the film, resulting in a surface morphology
with smaller triangles and lower relative height. The root-mean-
squared fluctuation of the surface atoms height is defined as surface
roughness. Fig. 5 shows the Cu and Ag film surface roughness of
the bilayer as a function of the applied strain. The Cu film sur-
face has a larger roughness than the Ag film surface at the yield
strain (ε = 7.3%), due to the preferred nucleation of dislocations
in the Cu film. And then the values of Cu and Ag surface rough-
ness decrease rapidly with the increase of strain until the same
level.
The evolution of SF atoms proportion in the Cu/Ag bilayer film at
ε = 7.3% is plotted in Fig. 6. During the tension of the Cu/Ag bilayer
film, SFs nucleate and propagate firstly in the Cu film in a short
time, followed by the SFs nucleation in the Ag film. As a result, SF
atoms proportion in the Cu film is far higher than that in the Ag
film at the initial stage of relaxation, and the value of total pro-
portion of SF atoms in the Cu/Ag bilayer film is between them. As
the strain increases, SF atoms proportion begins to decrease until a
stable state. The shear stress is the reason of SFs nucleation, and its
response can be divided into five regions over the time as shown in
Fig. 6.
Region (I): SF atoms in the Cu film suddenly increase, and shear
stress decreases, corresponding to the nucleation of a large number
of partial dislocations.
Region (II): the SFs atoms proportion in the Cu film sharply
decreases while that in the Ag film slowly increases, the former
is the major one, and the shear stress suddenly increases since it
cannot be effectively released.
Region (III): with the increase of SFs atoms proportion in the Ag
film, the latter becomes the major one and shear stress suddenly
decreases.
Strain ε Strain rateε̇
1]aCu 10−2 , 10−3 , 10−4
1]aAg 2–20%
1 1]aCu 10−2
1 1]˛Ag 10−2
452 L. Yuan et al. / Applied Surface Science 282 (2013) 450–455

Fig. 2. Dislocations nucleation and propagation in the Cu/Ag bilayer film during the relaxation at different equal biaxial tensile strains: (a) ε = 7.3% and (b) ε = 8%.

Fig. 3. Deformation defects in the Cu/Ag bilayer film after relaxation at ε = 7.5%: (a) top view of the single Cu atom layer in the interface and (b) perspective view of the
bilayer film with only defect atoms visible.

Region (IV): with the appearance and disappearance of the SFs,
the shear stress fluctuates;
Region (V): after relaxation of the film, the SFs and the level of
shear stress are essentially constant.
Fig. 7 compares the proportion evolution of SF atoms in the
Cu/Ag bilayer film, Cu film and Ag film subjected to the same strain
ε = 10%. A large number of SFs nucleate in both of the Ag film and Cu
film at the initial stage of relaxation, and the SF atoms proportion
in the monolayer film is about 2 times larger than that in the Cu/Ag
bilayer film. The reason is that the bilayer film interface will pre-
vent the initial SFs from extending into the Ag layer seriously. As
the relaxation evolution continues, the SF atoms proportion in the
monolayer film drastically decreases, while that in the bilayer film
slowly decreases, and finally both of them reach the same level. It
is shown that the interface plays a significant role in preventing the
evolution of defects just at the initial stage. With further relaxation,
the hindrance effect of the interface gradually weakens and does
not work to the final development of SFs almost. The appearing
time of SFs in the Cu/Ag bilayer film and Ag film is almost simul-
taneous, while the Cu film has a hysteresis, resulting in a lower
level of yield strain in the Cu film. The corresponding yield strain
value has a qualitative sequence of Cu/Ag bilayer film < Ag film < Cu
film.
Fig. 8 compares the evolution of the proportion of atoms in
the FCC structure and SFs in the Cu/Ag bilayer film after the ten-
sile steady state. The SFs fraction can characterize the mechanical
response of the film, which can be divided into five different
regions:
Elastic deformation strain region (I): ε < 7.3%, no defects;
 L. Yuan et al. / Applied Surface Science 282 (2013) 450–455 453

Fig. 4. Atomic morphology of the Cu and Ag free surfaces of the Cu/Ag bilayer film after relaxation at different equal biaxial tensile strains: (a) ε = 7.3% and (b) ε = 10%.

Critical strain region (II): 7.3% ≤ ε ≤ 7.4%, the elastic deformation
transforms to plastic deformation, corresponding to the rapid
increasing of SF atoms fraction;
Initial plastic deformation strain region (III): 7.4% < ε ≤ 8%, the SF
fraction decreases slowly;
Subsequence plastic deformation strain region (IV): 8% < ε ≤ 12%,
the SF fraction rises slowly;
High strain region (V): ε > 12%, SF fraction has a slight fluctuation.
Fig. 9 compares the SF atoms proportion in the Cu/Ag bilayer
film at three different strain rates. It indicates that the value
of the yield strain is 7.3% at high strain rate (ε̇ = 10−2 ps−1 ),
while 7.6% at lower strain rate (ε̇ = 10−3 ps−1 and 10−4 ps−1 ).
It also shows that at high strain rate plastic deformation occurs
earlier, which is consistent with the conclusion achieved by
observing the surface morphology under different strain rates.
The SF atoms proportion increases with the strain at the high
strain rate, while the rule is reversed at the low strain rate. The
smaller the strain rate is, the faster the SF atoms proportion
decreases.

Fig. 5. Dependence on strain of surface roughness of the Cu/Ag bilayer film after Fig. 6. Evolution of the proportion of SF atoms and shear stress in the Cu/Ag bilayer
relaxation. film at ε = 7.3%.
454 L. Yuan et al. / Applied Surface Science 282 (2013) 450–455

and different strain rates was studied using MD simulations. The

following conclusions are drawn:

(1) Dislocations are prone to nucleate at the interface of the Cu/Ag

bilayer film, and then propagate toward the free surface. With
the increase of strain, dislocations also nucleate at free sur-
face and the interior. Defect types include partial dislocations,
intrinsic stacking faults, accompanying with some extrinsic
stacking fault and stacking fault tetrahedra which just occurs
at the interface and extends to the Cu layer.
(2) Surface roughness of Cu/Ag bilayer film reaches the maxi-
mum value at the yield strain, and the roughness rapidly
decreases with the increase of strain. The mechanical response
can be divided into five regions according to the strain: Elastic
deformation strain region, critical strain region, initial plas-
tic deformation strain region, subsequence plastic deformation
strain region and high strain region. The corresponding yield
strain value has the relation of Cu/Ag bilayer film < Ag film < Cu
Fig. 7. Comparison of the proportion of SF atoms in the Cu/Ag bilayer film, Cu film
film.
and Ag film at ε = 10%.
(3) Atoms in stacking faults increase with the strain at the high
strain rate, while the rule is reversed at the low strain rate.
The smaller the strain rate is, the faster stacking fault atoms
proportion decreases.

Acknowledgements

This work is sponsored by the Seventh Framework Program of

the European Community for Research (Grant No. CP-FP 213600-
2 M3-2S), the National Science Foundation of China (Grant No.
51175110) and the Fundamental Research Funds for the Central
Universities (Grant No. HIT.KLOF.2010006).

References

[1] K.J. Hemker, W.N. Sharpe, Microscale characterization of mechanical proper-

ties, Annual Review of Materials Research 37 (2007) 93–126.
[2] R. Agrawal, H.D. Espinosa, Multiscale experiments: state of the art and
Fig. 8. Evolution of the proportion of atoms in the FCC structure and SFs in the remaining challenges, Journal of Engineering Materials and Technology 131
tensile steady state. (2009) 041208.
[3] H. Van Swygenhoven, Grain boundaries and dislocations, Science 296 (2002)
66–67.
[4] X. Li, Y. Wei, L. Lu, K. Lu, H. Gao, Dislocation nucleation governed softening and
maximum strength in nano-twinned metals, Nature 464 (2010) 877–880.
[5] J. Li, S. Sarkar, W.T. Cox, T.J. Lenosky, E. Bitzek, Y.Z. Wang, Diffusive molecular
dynamics and its application to nanoindentation and sintering, Physical Review
B 84 (2011) 054103.
[6] V. Vijayaraghavan, C.H. Wong, Temperature, defect and size effect on the elas-
tic properties of imperfectly straight carbon nanotubes by using molecular
dynamics simulation, Computation Materials Science 71 (2013) 184–191.
[7] I. Szlufarska, Atomistic simulations of nanoindentation, Materials Today 9
(2006) 42–50.
[8] M.A. Lodes, A. Hartmaier, M. Göken, K. Durst, Influence of dislocation den-
sity on the pop-in behavior and indentation size effect in CaF2 single crystals:
experiments and molecular dynamics simulations, Acta Materialia 59 (2011)
4264–4273.
[9] I. Shabib, R.E. Miller, A molecular dynamics study of twin width, grain size and
temperature effects on the toughness of 2D-columnar nanotwinned copper,
Modelling and Simulation in Materials Science 17 (2009) 055009.
[10] T.H. Fang, W.J. Chang, C.I. Weng, Nanoindentation and nanomachining charac-
teristics of gold and platinum thin films, Materials Science and Engineering A
430 (2006) 332–340.
[11] W.Y. Chang, T.H. Fang, S.J. Lin, J.J. Huang, Nanoindentation response of nickel
surface using molecular dynamics simulation, Modelling and Simulation 36
(2010) 815–822.
[12] S. Amaya-Roncancio, D.F. Arias-Mateus, M.M. Gomez-Hermida, J.C. Riano-
Fig. 9. Comparison of the proportion of atoms in SFs in the Cu/Ag bilayer film at Rojas, E. Restrepo-Parra, Molecular dynamics simulations of the temperature
three different strain rates. effect in the hardness on Cr and CrN films, Applied Surface Science 258 (2012)
4473–4477.
[13] S.H. Garofalini, S.H. Zhang, Molecular dynamics simulations of the effect of
4. Conclusions the composition of the intergranular film on fracture in Si3 N4 , Journal of the
American Ceramic Society 93 (2010) 235–240.
[14] S. Xu, Y.F. Guo, Z.D. Wang, Deformation mechanism of the single-crystalline
The deformation behavior of the Cu/Ag bilayer film, Cu film and nano-Cu films: molecular dynamics simulation, Computation Materials Science
Ag film subjected to the equal biaxial tension at different strains 67 (2013) 140–145.
 L. Yuan et al. / Applied Surface Science 282 (2013) 450–455
[15] K. Kolluri, M.R. Gungor, D. Maroudas, Atomic-scale analysis of defect dynamics
and strain relaxation mechanisms in biaxially strained ultrathin films of face-
centered cubic metals, Journal of Applied Physics 103 (2008) 123517.
[16] A.M. He, J.L. Shao, P. Wang, C.S. Qin, Plastic deformation of single-crystalline
copper films with surface orientation [0 0 1]: molecular dynamics simulations,
Acta Physica Sinica 59 (2010) 8836–8842.
[17] P.T. Sprunger, E. Lægsgaard, F. Besenbacher, Growth of ag on cu(1 0 0) studied by
stm: from surface alloying to ag superstructures, Physical Review B 54 (1996)
8163–8171.
[18] I. Meunier, G. Tréglia, B. Legrand, R. Tétot, B. Aufray, J.M. Gay, Molecular dynam-
ics simulations for the Ag/Cu(1 1 1) system: from segregated to constitutive
interfacial vacancies, Applied Surface Science 162/163 (2000) 219–226.
455
[19] Y. Mishin, M.J. Mehl, D.A. Papaconstantopoulos, A.F. Voter, J.D. Kress,
Structural stability and lattice defects in copper: ab initio, tight-
binding, and embedded-atom calculations, Physical Review B 63 (2001)
224106.
[20] P.L. Williams, Y. Mishin, J.C. Hamilton, An embedded-atom potential for the
Cu–Ag system, Modelling and Simulation in Materials Science 14 (2006)
817–833.
[21] S.J. Plimpton, Fast parallel algorithms for short-range molecular dynamics,
Journal of Computational Physics 117 (1995) 1–19.
[22] G.J. Ackland, A.P. Jones, Applications of local crystal structure meas-
ures in experiment and simulation, Physical Review B 73 (2006)
054104.