JMEPEG (2013) 22:2437–2445 ASM International

DOI: 10.1007/s11665-013-0541-z 1059-9495/$19.00

Parametric Study of Metal/Polymer Multilayer Coatings

for Temperature Wrinkling Prediction
Lihong Zhang, Anne Marie Habraken, Amine Ben Bettaieb, and Laurent Duchêne

(Submitted November 13, 2012; in revised form March 11, 2013; published online April 17, 2013)

This article presents an analytic model for the prediction of wrinkling occurring in metal/polymer coatings
under particular conditions. Owing to different thermal expansion coefficients (TECs) of the substrate and
the different coating layers, temperature variation can induce a compressive stress in the coating. The
wrinkling is the material response to the instability caused by this compressive stress. In this study, a
reference case was selected: a 0.27-mm-thick steel sheet with a 5-lm-thick polymer layer and, on top of it, a
thin aluminum film of 50 nm in thickness. For this reference case, it was observed and predicted by the
model that an increase in temperature yielded to the wrinkling of the thin aluminum film. The geometry of
the multilayer coating and the properties of the constituent materials are factors able to promote or prevent
the wrinkle. To better understand and predict their effects, a sensitivity analysis was carried out with the
proposed analytic model. A special attention was devoted to the temperature when wrinkling occurs. The
key parameters having a significant influence on the wrinkling temperature were identified. It is concluded
that the elastic modulus of the thin aluminum film and that of the polymer, the TEC of the thin film, and the
initial stress induced during the processing of the multilayer system all had a significant influence on the
wrinkling temperature.

wrinkling has a drastic negative effect on the targeted property

Keywords coating, metallic film, polymer, wrinkling
1. Introduction
With an ever-increasing number of industrial applications,
coatings play a significant role. They can be used to protect the
substrate, to infuse new properties to the surface of the material,
or to enhance these properties. In the application regarded in
this study, the coating is used to obtain a surface able to reflect
efficiently the light. In this respect, the quality of the surface in
terms of roughness, regularity, smoothness… is very important.
The multilayer system investigated consists in a substrate made
of a steel sheet with a thickness of 0.27 mm, the first coating
layer is a polymer having a thickness of 5 lm deposited by roll
coating. The final layer which permits to obtain the desired
property is a thin film made of Al6061 aluminum alloy with
50 nm in thickness obtained by magnetron sputtering.
Under particular external conditions, a compressive stress
can be generated in the thin aluminum film. Owing to larger
stiffness of the latter compared with the underlying polymer,
the compressive stress yields to instability of the film which can
lead to wrinkling. Wrinkling appears on the surface of the
material as a pattern of small wavelength waves. Obviously, the
Lihong Zhang, Amine Ben Bettaieb, and Laurent Duchêne,
ARGENCO Department, MS2F Division, University of Liège, Chemin
des Chevreuils 1, Liege 4000, Belgium; and Anne Marie Habraken,
ARGENCO Department, MS2F Division, University of Liège, Chemin
des Chevreuils 1, Liege 4000, Belgium; and F.R.S.—FNRS Fonds de
la Recherche Scientifique, Bruxelles, Belgium. Contact e-mail:
l.duchene@ulg.ac.be.
of the material surface, i.e., the reflection of light. Therefore,
the purpose of this article is to explore the metal/polymer
multilayer-coated steel sheets and particularly the effects of the
properties of the coating materials on the wrinkling phenom-
enon. In this respect, a parametric study was performed with the
objective of providing guidelines to manufacturers to avoid
wrinkling during the production and to improve the life of their
multilayer-coated steel sheets.
Owing to the larger thermal expansion coefficients (TECs)
of the coating materials (aluminum and polymer) compared
with the steel substrate, the detrimental compressive stress can
develop in the coating when the temperature of the multilayer
material increases (Ref 1, 2). It must be noted that other
external conditions may generate the compressive stress, e.g.,
the deposition technique, in particular, humidity conditions…
(the latter not being studied in this article).
The wrinkling phenomenon is receiving an increasing
attention because of the important uses of polymer coatings in
many industrial applications. Many attempts to model the
wrinkling phenomenon in metal/polymer coatings during the
heating of multilayer materials have been done. In a previous
study (Ref 3), the authors investigated the modeling of a two-
layer coating system using the critical stress equations based on
the work of Allen (Ref 4), Chen et al. (Ref 5), Huang (Ref 6) and
Yoo et al. (Ref 7). A critical compressive stress was determined
for the metal/polymer system from stability considerations.
When the compressive stress resulting from, among others, the
increase in temperature reaches the critical stress, the wrinkling
criterion is fulfilled. In that article, the authors compared the
different analytic predictions to finite element results.
The present article is devoted to a parametric study of the
thermally induced wrinkle in a metal/polymer coating system.
The temperature when wrinkling takes place is determined by

Journal of Materials Engineering and Performance Volume 22(9) September 2013—2437

the model and the influence of the coating material parameters
on this wrinkling temperature is assessed.
To summarize, the objectives of this article are twofold. In a
first stage, based on previous studies, a predictive tool is
developed to determine the wrinkling temperature of the
multilayer system according to the properties of the constitu-
ents. In a second stage, a sensitivity study is performed to
assess the influence of different parameters on the wrinkling
temperature. These two objectives will guide our industrial
partner to assess and improve the quality of its products thanks
to a better knowledge of the wrinkling temperature and the key
influential parameters on the wrinkling temperature.
However, to define precisely the context of our research
work, it must be mentioned that the wrinkling is not always
a detrimental phenomenon. Indeed, the wrinkling can be used
to obtain specific properties of the surface of the multilayer
system. In Ref 8, the wrinkling permits to tune the optical
properties of a cavity by modulating the effective refractive
index of the upper layer, while in Sabbah et al. (Ref 9), the
wrinkling phenomenon was used to develop superhydropho-
bic surfaces. These specific applications are possible thanks
to a thorough knowledge of the wrinkling characteris-
tics (amplitude, wavelength, orientation…) as proposed in
Ref 10, 11.
In the next section, the method based on an analytic
formulation to predict the wrinkling is briefly described [further
details can be found in our previous article (Ref 3)]. Section 3 is
devoted to the parametric study. In a first stage, the analytic
model is applied to derive the wrinkling temperature. Then, the
relevant parameters for our study are determined and their
effects are assessed successively in sections 3.3-3.8. The results
are discussed in section 4, and finally, general conclusions are
drawn. In the following, the subscripts f, p and s refer to the
different layers, i.e., the thin metal film, the polymer coating
and the steel substrate, respectively. The subscript w is related
to the wrinkled state.
2. Analytic Model
In order to predict the wrinkling temperature by an analytic
model, the critical stress of wrinkle and the current stress in the
thin film are required. Wrinkling appears when the compressive
stress resulting from a mismatch of TEC between the substrate
and the capping layer of the system during heating exceeds (in
absolute value) a critical value. In several applications of two-
layer coatings, the top layer is much stiffer than the adhesion
layer. If this stiffness mismatch increases, then the critical stress
decreases, and the wrinkle phenomenon is more likely to
appear. Since the metallic top layer has a yield stress much
larger than that of the adhesion layer, the thin top layer remains
in the elastic regime during heating and eventually during
wrinkling.
Concerning the underlying adhesion layer, as it is made of
polymer, its mechanical behavior can correspond to one of the
three following regimes: elastic (Ref 4, 5, 12), viscoelastic
(Ref 6, 7, 13), or viscous (Ref 13-15). At low temperatures, the
polymer is dominated by an elastic behavior and the wrinkling
can be described by the free energy approach (Ref 7). When the
temperature is raised slightly above the glass transition
2438—Volume 22(9) September 2013
temperature (Tg) of the polymer (which is 45 C for the
selected polymer), its behavior changes from an elastic regime
to a viscoelastic rubbery regime, introducing a drastic change in
its TEC and its stiffness. In the latter regime of the polymer, the
rigorous modeling of the wrinkling phenomenon is very
complicated. If the temperature is further raised to a higher
range, then the polymer changes into a viscously flow state.
The viscous behavior dominates, and the wrinkling can be
described by a kinetic approach (Ref 16).
In this study, the temperature is kept near Tg, corresponding
to a viscoelastic regime for the polymer. However, a temper-
ature and strain rate-dependent elastic modulus is used to model
the mechanical behavior of the polymer (see Ref 3 for a
detailed description of the polymer modeling approach and for
values of the temperature and strain rate-dependent elastic
modulus). According to this assumption, an analytic formula-
tion based on the free energy approach (Ref 7) for an elastic
regime of the polymer can be used. The experimental
characterization test used to derive this temperature and strain
rate-dependent modulus is a dynamic mechanical thermal
analysis (DMTA) diagram.
Based on the assumptions described above, the critical stress
related to the stability of the multilayer coating can be calculated by
applying the analytic model (Ref 4-6) presented in section 2.1.
Besides, the thermally induced compressive stress can be calcu-
lated according to the approach of Townsen et al. (Ref 17) as shown
in section 2.2. Finally, the comparison of the critical stress to the
temperature-induced stress provides a wrinkling criterion allowing
the determination of the wrinkling temperature Tw.
2.1 Stability of the Multilayer Coating
Figure 1 illustrates the structure under consideration in a
schematic wrinkled configuration: a thin aluminum film of
thickness hf is bonded to a polymer layer having a thickness of
hp, which in turn is bonded to a steel substrate of thickness hs.
With regard to its stiffness and thickness, the steel substrate is
assumed perfectly stiff and flat. According to the above
assumptions, both coating layers are assumed to behave in the
elastic regime (with a temperature and strain rate dependence
for the polymer). Therefore, the free energy approach (Ref 7)
can be used to calculate the critical stress leading to the
instability of the thin metal film which is modeled by the
nonlinear von Karman plate theory (Ref 18).
The bi-layer problem can be analytically solved under some
particular conditions. Departing from a plane strain hypothesis,
for hp/hf fi ¥, a linear stability analysis permits to obtain the
wrinkling critical stress rc according to Chen et al. (Ref 5):
λ
Thin metal film hf
2A
Polymer hp
Steel hs
Fig. 1 Schematic representation of the multilayer system in the
wrinkled state with definition of k, A, hs, hp and hf
Journal of Materials Engineering and Performance
   0  12=3
rc 1  m2f 1 @3Ep 1  m2f A
¼   ; ðEq 1Þ
Ef 4 Ef 1  m2
p where DT = T  T0 is the temperature increase.
where E is the YoungÕs modulus and m is the PoissonÕs ratio
of the film or the polymer according to the subscript f or p.
Note that Huang (Ref 6) gave another expression for the criti-
cal stress, which is however equivalent to Eq 1 in identical
conditions.
It must be noted that, in Eq 1, the critical stress is
independent of the thickness of the thin metal film and the
polymer because of the assumption hp/hf fi ¥, which is
valid for the studied case, as we have hp/hf = 5 lm/
50 nm = 100.
The developments leading to Eq 1 assumed an elastic
regime for both metallic and polymer layers. However, it must
be bore in mind that the viscosity of the polymer is taken into
account through the variation of the elastic modulus Ep with the
temperature and the strain rate (see section 3.4).
A rapid decrease of the elastic modulus is often observed
when the temperature rises. Thus, a fast decrease of the critical
stress is induced by the heating of the coating. Consequently, a
final temperature close to Tg is often sufficient to induce the
wrinkling phenomenon (see section 3).
2.2 Thermal Stress
For a multilayer sheet constitutive of materials having
different YoungÕs moduli E, PoissonÕs ratios m, and thicknesses
h, Townsen et al. (Ref 17) proposed an approach assuming that,
before the instability occurs, the surface of the coating is large
enough compared with its thickness so that it can be considered
planar. As, additionally, the curvature of the sheet is neglected,
the in-plane thermal stress in the metal film generated by a
temperature increase from T0 to T can be calculated from the
equilibrium of the system and the compatibility of the different
layers (Ref 17, 19, 20). It results from the difference between
the weighted average TEC a  of the multilayer system and the
TEC of the metal film af:
ZT
Ef
rf ¼   af ÞdT
ða ðEq 2Þ
1  mf
T0
For the determination of a ; accurate information about the
evolution of the TEC of the polymer ap as a function of the
temperature was not available for the studied polymer. This
could lead to inaccurate results since the TEC of the polymer
is known to vary considerably in the temperature range inves-
tigated (around Tg). However, knowing the significantly larger
thickness and elastic modulus of the steel compared with the
two coating materials, the weighted average TEC a can be re-
placed with a good approximation by the TEC of the steel as:
P
a E h =ð1  mi Þ
¼ Pi i i
a  as ðEq 3Þ
Ei hi =ð1  mi Þ
where both sums range for i = f, p, s, respectively, for the
three constituent materials of the system. Therefore, with the
TEC of the two metallic layers (aluminum and steel) being
rather constant in the investigated temperature range, the in-
plane thermal stress in the film reduces to
Journal of Materials Engineering and Performance
Ef
rf ¼ ðas  af ÞDT ðEq 4Þ
1  mf
3. Parametric Study
3.1 Determination of the Wrinkling Temperature
The developments presented in sections 2.1 and 2.2 permitted
to determine the wrinkling critical stress and the temperature-
induced stress in the thin metal film, respectively. The values of
these stresses are plotted as a function of the temperature in
Fig. 2. As already mentioned, owing to a decrease of the stiffness
of the polymer, the critical stress rapidly decreases (in absolute
value) when the temperature rises. On the contrary, the thermal
stress increases gradually when the temperature increases
according to Eq 4. The intersection of these two curves is the
condition for the instability to occur; therefore, it defines the
wrinkling temperature, which is 59.12 C in this case.
It must be noted that, owing to its deposition process, an
initial internal (or residual) compressive stress arises in the
metallic thin film (Ref 21). This internal stress rini must be
added to the thermal stress for the determination of the
wrinkling temperature. As the actual value of the residual stress
for the studied case is not (yet) available, a low value of
20 MPa was chosen as a reference. The effect of this value on
the wrinkling temperature was analyzed in the parametric study
(see section 3.3).
The present study and especially the curves of Fig. 2 are
focused on a reference case. Table 1 details the mechanical
properties, the TEC, the thicknesses, and the internal stresses of
the different layers for this reference case. For the multilayer
coating investigated in this article, the wavelength of the
wrinkling (see Fig. 1) has a value around 5320 nm.
3.2 Relevant Parameters for the Study
Working on the three-layer system: thin metal film/polymer/
steel, any of the 15 entries of Table 1 could be considered for
the parametric study. However, assuming that the parameters
related to the steel sheet are fixed, the current study focuses on
the two coating layers, which reduces the parametric study to
10 variables.
-1000
MPa Critical stress
Thermal stress and initial stress (-20MPa)
-100
Tw=59.12°C
T (°C)
-10
40 50 60 70 80 90
Fig. 2 Determination of the wrinkling temperature
Volume 22(9) September 2013—2439
Table 1 Mechanical properties, TEC, thicknesses, and internal stresses of the multilayer system in the reference case
(from Ref 3)
Layer E (GPa) m a (1026/°C) h rini (MPa)

Steel 210 0.3 12 0.27 mm 0

Polymer Variable 0.43 90 5 lm 0
Metal film (Al) 70 0.33 24 50 nm 20

70 Tw (°C) Eq 1 and 4. Furthermore, as already mentioned and detailed in

60 wrinkle
50
40
30
no wrinkle
20
10 σini (MPa)
0
0 -100 -200 -300 -400
Fig. 3 Wrinkling temperature vs. the initial stress of the thin metal
film
As discussed in section 2.2, the steel dominates the thermal
expansion of the multilayer sheet, and, as shown by Eq 4, the
thermal stress in the film is significantly influenced by Ef, mf, af,
and as, where as was already eliminated from the study. For the
wrinkling critical stress, according to Eq 1, there are just four
influential parameters: Ef, mf, Ep, and mp. Besides, no internal
stress is expected to develop in the polymer and, in addition,
according to the model, it would have no influence on the
wrinkling temperature.
Finally, only the effect of six parameters, namely Ef, mf, Ep, mp,
af, and the internal stress in the film rini, on the wrinkling
phenomenon of the two-layer coating system is assessed. Note that,
for the developed analytic model, the thicknesses of the polymer
and the thin metal film are not supposed to affect the wrinkling
temperature as long as the condition hp/hf fi ¥ is fulfilled.
The ranges of variation for the different parameters were
chosen to represent widely used materials and to cover realistic
values. The effect of dispersion in the determination of YoungÕs
modulus with respect to its reference value was also checked. The
following subsections are dedicated to the analysis of the influence
of the selected parameters separately (except for the internal stress
coupling of which with other parameters is also studied).
3.3 Influence of the Residual Stress in the Film rini
According to the method used to determine the wrinkling
temperature Tw (see Fig. 2), if the internal stress in the film rini is
increased (in absolute value), the thermal and internal stress curve
(continuous line) moves upward, which corresponds to a
decrease of Tw. By repeating the computation for several values
of rini, Fig. 3 is obtained. It shows the evolution of the wrinkling
temperature Tw as a function of the internal stress in the film.
3.4 Temperature and Strain Rate Dependant Elastic
Modulus of the Polymer Ep
The influence of Ep on the wrinkling temperature can be
obtained according to the method proposed in section 3.1 using
Ref 3, the elastic modulus of the polymer Ep was determined
from the experimental DMTA as a function of the temperature
and the strain rate prevailing when the wrinkling is expected to
occur. Therefore, the dependence of the wrinkling temperature
on Ep can be associated in a dependence on the temperature and
the strain rate.
In addition, during the wrinkling process, the multilayer
system is solely submitted to an increase in temperature. For
that particular loading, the strain rate can be calculated. Indeed,
reasoning for the one dimensional case, the strain in the
ith layer induced by the thermal mismatch in the multilayer
system is:
 
LF
ei ¼ ln ; ðEq 5Þ
Li
where for the current temperature, LF is the final length of
the multilayer system and Li is the length of the ith layer in
the stress free state. In the case of the studied two layer coat-
ing where the steel substrate dominates the mechanical behav-
ior, the strain in the polymer layer at the temperature T
(assuming no thermal mismatch at T0) can be obtained:
 
as ðT  T 0 Þþ1
ep ¼ ln ðEq 6Þ
ap ðT  T 0 Þþ1
Then, the strain rate is:
as T_ ap T_
e_ p ¼  ; ðEq 7Þ
as ðT  T 0 Þþ1 ap ðT  T 0 Þþ1
where ap and as are assumed constant in the studied tempera-
ture range. In the investigated application, the maximum in-
crease of temperature (T  T0) is limited to 70 C, which
yields to the approximations as(T  T0)  1 and ap(T 
T0)  1. Finally, the strain rate in the polymer layer can be
given by:
 
e_ p ¼ as  ap T_ ðEq 8Þ
Consequently, the strain rate dependence of the elastic
modulus of the polymer Ep can be related to the temperature
rate. Through Ep, the wrinkling temperature can be expressed
as a function of the temperature history of the multilayer
system. Figure 4 shows the curve of the wrinkling temperature
versus the temperature rate, while Table 2 summarizes the
effect of the temperature rate.
3.5 PoissonÕs Ratio of the Polymer mp
Table 3 gives possible variations of mp and their effect on Tw.
For PoissonÕs ratios of the polymer ranging from 0.38 to 0.45,
Tw varies of 0.38 C. It can be considered that there is no
significant influence of mp on Tw.

2440—Volume 22(9) September 2013 Journal of Materials Engineering and Performance

3.6 YoungÕs Modulus of the Metal Film Ef YoungÕs modulus increases. For a higher initial stress
(rini = 200 MPa), the same range for Ef introduces a
Table 4 presents the values of YoungÕs modulus Ef of
variation of only about 1.5 C for Tw. In this case, Tw increases
several metals that could be used for the thin film [Sn (Ref 22),
slightly when YoungÕs modulus increases. The influence of the
Al (Ref 23, 24), Ag (Ref 25), Ti (Ref 23, 26), Cu (Ref 23),
elastic modulus of the film is notably reduced when the initial
stainless steel (Ref 23), Cr (Ref 27), and Mo (Ref 24)].
stress is increased.
According to this selection, the values of Ef for the parametric
When Ef varies between 67 and 73 GPa (corresponding to
study were chosen from 40 to 350 GPa. Besides, a reduced
9% of relative variation), Tw variation is 0.26 C for
range (67-73 GPa) was further analyzed to check the influence
rini = 20 MPa and 0.12 C for rini = 200 MPa. It can be
of the modulus dispersion for the aluminum reference case.
concluded that the dispersion of Ef for one material has no
Using magnetron sputtering for the deposition of the aluminum
influence on Tw, independently of the value of the initial stress.
thin film, nanosized grains are generally obtained which can
As mentioned in section 3.3 and Fig. 3, the initial stress has
modify some mechanical properties. Furthermore, the films
a quite large influence on the wrinkling temperature. In
obtained by such a synthesis may be porous which can also
addition, Fig. 5 shows that this effect is larger when YoungÕs
justify the study of a slight variation of YoungÕs modulus
modulus of the film is low. For instance, when Ef = 40 GPa,
around the average value.
the difference in Tw is 15.25 C for rini changing from 20 to
Tables 5a, b, and 6a, b summarize the effect of YoungÕs
200 MPa.
modulus on the wrinkling temperature for the two selected
ranges and for two levels of initial stress. Figures 5 and 6 show
Tw as a function of Ef in the total range (40-350 GPa) and in the 3.7 PoissonÕs Ratio of the Metal Film mf
reduced range (67-73 GPa), respectively.
For the reference level of initial stress (rini = 20 MPa), Table 7 shows the evolution of the wrinkling temperature
when Ef ranges from 40 to 350 GPa (corresponding to a for different values of mf. It appears that a change in PoissonÕs
relative variation from 43 up to 400% of the reference value), ratio of the thin metal film from 0.28 to 0.35 induces a variation
Tw varies of about 11 C. It is observed that Tw decreases when of Tw of only 0.45 C. This observation emphasizes the fact
that mf value does not affect the wrinkling temperature.

Tw (°C) 3.8 Thermal Expansion Coefficient of the Metal Film af

80
wrinkle
Table 8 presents the value of the TEC of several metals: Sn
70 (Ref 28), Al (Ref 23), Ag (Ref 29), Ti (Ref 28), Cu (Ref 23),
stainless steel 304, and Mo (Ref 24). Table 9a, b and Fig. 7
60 show the dependence of Tw on af. The differential thermal
expansion of the thin metal film with respect to the steel
50 no wrinkle
substrate is at the origin of the wrinkling phenomenon. It was
40
therefore expected that af has a significant influence on Tw.
Temperature rate (°C/min) Indeed, as presented in Fig. 7 and Table 9a, the influence of af
30 is very large for a low initial stress (rini = 20 MPa).
1 10 100 1000 10000 However, as was observed for Ef, when the initial stress
becomes higher (200 MPa), the influence of af on Tw is
Fig. 4 Wrinkling temperature vs. the temperature rate during the reduced.
heating of the multilayer system

Table 2 Effect of the elastic modulus of the polymer (related to the strain rate and the temperature rate) on the wrin-
kling temperature Tw in the two layer coating (bold values correspond to the reference case)
T_ (°C/min) 1 3 7.69 30 76.9 769.2

e_ p;e 1.3 9 106 3.9 3 1026 1.0 9 105 3.9 9 105 1.0 9 104 1.0 9 103
Tw (C) 58.16 59.12 60.04 62.79 64.95 68.96
_ _ 
T ðTÞref
ðT_ Þref
(%) 66.7 0 156 900 2463 25540
(Tw  (Tw)ref) (C) 0.96 0 0.92 3.67 5.83 9.84

Table 3 Effect of PoissonÕs ratio of the polymer on the wrinkling temperature Tw in the two layer coating (bold values
correspond to the reference case)
mp 0.38 0.4 0.41 0.42 0.43 0.44 0.45

Tw (C) 58.85 58.95 59.01 59.06 59.12 59.18 59.23

 
mp ðmp Þref
ðmp Þref (%) 11.63 6.98 4.65 2.33 0 2.33 4.65
(Tw  (Tw)ref) (C) 0.27 0.17 0.11 0.06 0 0.06 0.11

Journal of Materials Engineering and Performance Volume 22(9) September 2013—2441

Table 4 YoungÕs modulus Ef of different metals (bold values correspond to the reference case)
Metal Sn (Ref 22) Al (Ref 23, 24) Ag (Ref 25) Ti (Ref 23, 26) Cu (Ref 23) Stainless steel (Ref 23) Cr (Ref 27) Mo (Ref 24)

Ef (GPa) 50 70 87.3 110 120 205 279 343

Table 5 Effect of YoungÕs modulus of the thin film on the wrinkling temperature Tw in the two layer coating (a) for the
reference level of initial stress rini = 220 MPa and (b) for a higher level of initial stress rini = 2200 MPa
Ef (GPa) 40 60 70 80 120 200 350

(a) rini = 20 MPa

Tw (C) 61.3 59.56 59.12 58.68 57.06 54.28 50.36
 
Ef ðEf Þref
ðEf Þ (%) 42.9 14.3 0 14.3 71.4 186 400
ref

(Tw  (Tw)ref) (C) 2.18 0.44 0 0.44 2.06 4.84 8.76

(b) rini = 200 MPa
Tw (C) 46.05 46.79 47.01 47.18 47.55 47.72 47.51
 
Ef ðEf Þref
ðEf Þref (%) 42.9 14.3 0 14.3 71.4 186 400
 
Tw  ðTw ÞEf ¼70 GPa (C) 0.96 0.22 0 0.17 0.54 0.71 0.50

Bold values correspond to the reference case

Table 6 Effect of YoungÕs modulus of the thin film (in a reduced range) on the wrinkling temperature Tw in the two layer
coating (a) for the reference level of initial stress rini = 220 MPa; and (b) for a higher level of initial stress rini = 2200 MPa
Ef (GPa) 67 68 69 70 71 72 73

(a) rini = 20 MPa

Tw (C) 59.25 59.20 59.16 59.12 59.07 59.03 58.99
 
Ef ðEf Þref
ðEf Þ (%) 4.29 2.86 1.43 0 1.43 2.86 4.29
ref

(Tw  (Tw)ref) (C) 0.13 0.08 0.04 0 0.05 0.09 0.13

(b) rini = 200 MPa
Tw (C) 46.95 46.98 47.00 47.01 47.03 47.05 47.07
 
Ef ðEf Þref
ðEf Þref (%) 4.29 2.86 1.43 0 1.43 2.86 4.29
 
Tw  ðTw ÞEf ¼70 GPa (C) 0.06 0.03 0.01 0 0.02 0.04 0.06

Bold values correspond to the reference case

65 65 Tw (°C)
Tw (°C)

60 60 σini = -20MPa
σini = -20MPa

55 55

σini = -100MPa σini = -100MPa

50 50
σini = -200MPa σini = -200MPa
Ef (GPa) Ef (GPa)
45 45
0 50 100 150 200 250 300 350 67 68 69 70 71 72 73

Fig. 5 Wrinkling temperature vs. YoungÕs modulus of the thin film Fig. 6 Wrinkling temperature vs. YoungÕs modulus of the thin film
for three values of initial stress for three values of initial stress (reduced range)

4. Discussion It identifies the key factors according to their influence on the

wrinkling temperature.
In order to review the influence of the studied parameters, This analysis shows that the effects of the PoissonÕs ratios of
Table 10 summarizes the observations of the parametric study. the thin metal film mf and the polymer layer mp on the wrinkling

2442—Volume 22(9) September 2013 Journal of Materials Engineering and Performance

Table 7 Effect of PoissonÕs ratio of the film on the wrinkling temperature Tw in the two layer coating (bold values corre-
spond to the reference case)
mf 0.28 0.30 0.31 0.32 0.33 0.34 0.35

Tw (C) 
 59.43 59.30 59.25 59.18 59.12 59.05 58.98
mf ðmf Þref
ðmf Þref (%) 15.2 9.09 6.06 3.03 0 3.03 6.06
(Tw  (Tw)ref) (C) 0.31 0.18 0.13 0.06 0 0.07 0.14

Table 8 TEC af of different metals (bold values correspond to the reference case)
Metal Sn (Ref 28) Al (Ref 23) Ag (Ref 29) Ti (Ref 28) Cu (Ref 23) Stainless steel (304) Mo (Ref 24)

af (106/C) 22 24 19 8.6 17 16.9 5.0

Table 9 Effect of the TEC of the thin film on the wrinkling temperature Tw in the two layer coating (a) for the reference
level of initial stress rini = 220 MPa and (b) for a higher level of initial stress rini = 2200 MPa
af (1026/°C) 15 16 18 20 22 24 26

(a) rini = 20 MPa

w (C) 
T >90 84.98 67.45 63.05 60.23 59.12 58.16
af ðaf Þref
ðaf Þ (%) 37.5 33.3 25 16.7 8.3 0 8.3
ref

(Tw  (Tw)ref) (C) >30 25.86 8.33 3.93 1.11 0 0.96

10 12 14 18 22 24 26

(b) rini = 200 MPa

w (C)
T 48.21 48.04 47.87 47.53 47.19 47.01 46.84
af ðaf Þref
ðaf Þref Þ (%) 58.3 50 41.7 25 8.3 0 8.3
 
Tw  ðTw Þaf ¼24106 = C (C) 1.20 1.03 0.86 0.52 0.18 0 0.17

Bold values correspond to the reference case

Tw (°C) the wrinkling temperature (see Fig. 3). In addition, it also

80 modifies the effect of other parameters, i.e., the shape of the Tw-
σini =-20 MPa Ef curves (Fig. 5) and the Tw-af, curves (Fig. 7) are largely
70 σini =-50 MPa influenced by the value of rini.
In the parametric study, the YoungÕs modulus Ef corre-
60 sponding to the chosen material affected the prediction of the
wrinkling temperature. However, one must consider that
50 changing the material of the thin film also modifies other
σini =-200 MPa parameters such as mf and af. Therefore, while the effect of
40
PoissonÕs ratio can be disregarded, it is necessary to check the
α f (10-6 /°C)
30
values of Ef and af of the selected real materials to examine the
10 15 20 25 combined influence of these parameters. In this respect, Fig. 8
shows the surface of Tw as a function of Ef and af, which are
Fig. 7 Wrinkling temperature vs. the TEC of the thin metal film among the most influential parameters on Tw. For the com-
for three values of initial stress pleteness of the figure, the surface of Tw is plotted for two
different levels of initial stress in the film. The sticks in Fig. 8
locate the different metals which could be chosen as thin metal
temperature can be neglected. Contrarily, the TEC of the thin films according to their Ef and af values.
metal film af, its YoungÕs modulus Ef, the polymer elastic For the reference level of initial stress (20 MPa), the large
modulus Ep (related to T_ ) and the initial stress in the metal film effects of Ef and af are clearly observable in Fig. 8. When the
rini are predominant parameters in the wrinkling phenomenon. TEC of the thin film is increased, the thermal mismatch with the
The influence of Ef in the range 40-350 GPa on Tw is steel substrate (having a value of as = 12 9 106/C) increases,
noticeable (see Fig. 5), while a low dispersion of Ef for one and the wrinkling is more likely to appear, which leads to a
material has a very limited effect on Tw (see Fig. 6). The level lower wrinkling temperature. Similarly, when YoungÕs modulus
of initial stress in the thin film significantly alters the value of of the thin film is increased, the thermal mismatch between the

Journal of Materials Engineering and Performance Volume 22(9) September 2013—2443

Table 10 Summary of the sensitivity study
Study area
Reference Study area in % (with respect to the
Parameter value in absolute value reference value) Effect on Tw

rini (MPa) 20 350 to 0 100 to 1650 Strong (20 C)

T_ (through Ep) (C/min) 3 1-769.2 66.7 to 25540 Significant (10.8 C)
mp 0.43 0.38-0.45 11.6 to 4.7  (0.38 C)
No
Significant ð10:94 Þ if rini ¼ 20 MPa
Ef (GPa) 70 40-350 43 to 400
Weak ð1:67 Þ if rini ¼ 200 MPa
mf 0.33 0.28-0.35 15 to 6  (0.45 C) 
No
6 Strong ð > 30 Þ if rini ¼ 20 MPa
af (10 /C) 24 10-26 58.3 to 8.3
Weak ð1:37 Þ if rini ¼ 200 MPa

Fig. 8 Wrinkling temperature surface vs. the TEC and YoungÕs modulus of the thin film

different layers yields to an increased compressive stress
because of the larger stiffness of the film, which, in turn,
promotes the wrinkling. It can be concluded that, when
the initial stress is low, Ef and af are the key parameters for
the wrinkling due to their influence on the development of the
compressive thermal stress in the film.
For a high initial stress level in the thin metal film
(200 MPa), the compressive stress is present in the thin film
after its deposition, even without any thermal mismatch. The
wrinkling is then related to the capacity of the multilayer
system to sustain this compressive stress in a stable way. Tw is
therefore determined on the basis of the critical stress in the film
according to Eq 1, temperature dependence of which derives
from the temperature-dependent elastic modulus of the polymer
Ep. Consequently, for a high initial stress, it is observed that the
properties of the thin film have a reduced influence, while the
polymer properties, through their temperature dependence, play
an important role in the wrinkle development in the two-layer
coating.
5. Conclusions
In this study, an analytic model was developed to predict the
wrinkling temperature of a coating system consisting of a thin
metal film and a polymer layer deposited on a steel substrate.
The analytic model is briefly described, and a reference case is
presented. Then, a parametric study was performed to check the
influence of several input data such as the material properties of
the different layers and the initial stress in the thin film (owing
to the fabrication process). It is concluded that the identification
of the key parameters clearly depends on the value of the initial
stress.
In future studies, the internal stresses due to the coating
process will be determined experimentally, which will permit
us to increase the predictive capabilities of our analytic model.
Besides, the influence emphasized by Ref 30 of the temperature
increase on the value of the internal stress induced by the
magnetron sputtering process should also be taken into account.
In the present article, the TEC of the polymer ap was
assumed independent of the temperature, while it is known to
greatly vary above Tg. It should therefore be considered to
improve the model.
Acknowledgments
The authors thank the Walloon Region (Winnomat2 Dinosaure
project). The Belgian Scientific Research Fund F.R.S. - FNRS
which finances A.M.H., and the Belgian Sciences Policy (inter-
university attraction poles program IAP P7/21) are thanked for
their financial support. The authors would also thank their
industrial partner for this Winnomat2 project, namely AC&CS,
subsidiary of CRM group (previously AMLR, subsidiary of
ArcelorMittal).

2444—Volume 22(9) September 2013 Journal of Materials Engineering and Performance

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