Surface and Coatings Technology 125 (2000) 185189

www.elsevier.nl/locate/surfcoat

Mechanical behaviour of hard PVD multilayered coatings

E. Harry a, *, M. Ignat b, Y. Pauleau b, A. Rouzaud c, P. Juliet c
a Laboratoire des Sciences & Ingenierie des Surfaces, Universite Claude Bernard Lyon 1,
43 boulevard du 11 Novembre 1918, Bat. 305, F-69622 Villeurbanne, France
b ENSEEG, F-38402 Saint Martin dHe`res, France
c CEA, F-38054 Grenoble Cedex 9, France

Abstract
The aim of this work was to investigate the cracking behaviour and adhesion of tungstencarbon-based multilayered coatings
deposited on steel substrates by magnetron sputtering. Three-point bending experiments were performed on the coating-onsubstrate systems until failure of the film. The systems were also strained uniaxially with a microtensile device adapted to a
scanning electron microscope. The mechanical response is analysed from the evolution of the crack density in the coating and the
fracture toughness. The results show that the rupture properties of the multilayered coatings are correlated to the film thickness
and arrangement of the elementary layers. Scratch experiments on the systems revealed a strong adhesion of the multilayered
coatings on steel substrates, and delamination at layer interfaces. Thus, graded coatings appear to be more attractive for mechanical
applications. 2000 Elsevier Science S.A. All rights reserved.
Keywords: Coatings; Cracking; Multilayers; Tungsten; Tungstencarbon

1. Introduction
Tungsten carbide coatings prepared by chemical
vapour deposition or physical vapour deposition appear
to be attractive candidates for the protection of mechanical components (such as cutting tools) against wear or
erosion [1]. However, these hard coatings exhibit brittle
mechanical behaviour which can affect their reliability.
To improve the erosion or wear resistance of hard
coatings, a judicious combination of hardness and
toughness should be favourable. Hence, hard multilayered coatings based on a stacking arrangement of ductile
layers and hard layers have been developed [2,3].
Multilayered coatings produced by sputtering and composed of pure tungsten layers ( W ) and hard tungsten
carbon layers [ W(C )] were found to be very promising
erosion-resistant coatings for compressor blades in gas
turbine engines [2]. The performance of these protective
coatings appears to be governed by the cracking resistance and adhesion of the composites, and the by the
mechanical behaviour of the elementary layers. Harry
et al. reported that tungsten and W(C ) layers deposited
* Corresponding author. Tel: +33-4-72-44-83-06;
fax: +33-4-72-43-12-06;
E-mail address: harry@cismcun.univ-lyon1.fr ( E. Harry)

by magnetron sputtering have quite different mechanical

properties, since columnar tungsten films behave like a
ductile material compared with W(C ) films, which are
dense and brittle [4,5]. Indeed, tungsten layers exhibit a
fracture toughness close to 2 MPa m1/2 and appear to
adhere well to stainless steel substrates. By contrast, the
cracking resistance of W(C ) layers was found to be
about two times lower than that obtained for tungsten
layers; these films have also shown very poor adhesion
on stainless steel substrates. The mechanical behaviour
of multilayered coatings of this type layers has been
investigated, and was found to depend on the nature of
the layer at the interface between the substrate and the
coating. In particular, a columnar tunsgten interfacial
layer appears to limit delamination of the coatings,
through a contribution arising from motion of the
columns.
The aim of this work was to investigate the mechanical response of multilayered coatings of this type submitted to an elongation. This includes determination of
the critical deformation of the film corresponding to
crack onset, and determination of the fracture toughness
using an analytical approach. The fracture properties of
the films are discussed through a Weibull analysis and
the damage mechanisms examined with respect to coating architecture. Then, the adhesion of the multilayered
coatings is characterised qualitatively.

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E. Harry et al. / Surface and Coatings Technology 125 (2000) 185189

2. Experimental details
Coatings were deposited on stainless steel substrates
by direct-current reactive magnetron sputtering.
Experimental details of the procedure have been
reported previously [4,6 ]. The multilayered coatings are
based on the stacking arrangement of two or four
successive layers of tungsten ( W ) and tungstencarbon
[ W(C ) with 14 at% of carbon]. The bilayer and fourlayer coatings are named 2L-W(C )/W and 4L-W(C )/W,
respectively. These multilayered coatings, of thickness
ranging from 3.5 mm to 14 mm, are composed with a
columnar tungsten layer located at the substrate/coating
interface and a hard W(C ) top layer.
The films were submitted to three different types
of test:
$ three-point bending tests [7], to determine the
Youngs modulus and to detect the onset of cracking
of the coating;
$ uniaxial tensile tests performed in a scanning electron
microscope (SEM ), supplying some new information
in the analysis of the mechanical response of the
deposited materials [8]. These experiments permit us
to follow the evolution of the transverse crack density
in the films when the applied strain is increased; and
$ scratch tests performed under loads ranging from 0
to 100 N. The loading rate and displacement speed
of the indentor are 100 N min1 and 10 mm min1,
respectively. The objectives of this method are to
evaluate the adhesion of the coatings to the substrate
and to rank the coatings with respect to debonding
resistance.
3. Mechanical properties
The hardness of the multilayered coatings was measured by classical Vickers microindentations under 50 g
for films of thickness 14 mm. As a result, the effect of
the hardness of substrates covered with relatively thick
coatings can be neglected. The microhardness values lay
between 26 GPa for the four-layer coatings and 28 GPa
for the bilayer coatings. The microhardness of the
multilayered coatings was close to that of the material
deposited on top of the coating, i.e., W(C ) [4].
The residual stresses in the films were determined by
means of substrate curvature measurements before and
after deposition of the coatings, using the Stoney formula. The multilayered coatings are found to be in a
compressive state. The level of residual stress appears
to be similar for both types of multilayered coating, and
very high, close to 3 GPa, without any delamination
of the films.
The Youngs modulus of the coatings was determined
through three-point bending experiments, performed on
the substrate only and on the coated substrate. The
device used and the experimental procedure are

described elsewhere [5,7]. Assuming perfect adhesion of

the films on the substrates, when the sample is submitted
to an elastic bending, calculations derived from an
energy balance on the composite structure lead to the
following simple equation:
ts F F
2
1,
(1)
3tf F
1
where Es, ts and Ef, tf are the Youngs modulus and
thickness of the substrate and the film, respectively. F
1
and F are the forces which correspond to bending of
2
the substrate and the composite to the same deflection.
The parameter (F F )/F is determined experimentally,
2
1 1
and the films Youngs modulus is then deduced.
The experimental mean value of Youngs modulus is
around 391 GPa for the multilayered coatings, whatever
their architecture or thickness. This result shows that
the Youngs modulus of 2L-W(C )/W and 4L-W(C )/W
coatings is close to the tungsten bulk value [9].
Ef=Es

4. Cracking investigation
Techniques to determine fracture properties such as
the fracture toughness of bulk materials are not suitable
for determination of the same parameters in thin coatings. Therefore, new experimental methods have been
developed [8,10,11]. In our case, we first performed
three-point bending tests, and then in situ microtensile
tests, both to determine the fracture parameters and to
study the rupture properties of the coatings.
Investigations of this type on the elementary tungsten
and W(C ) layers have been carried out previously [5].
Then, the results obtained for the multilayered coatings
could be compared with those obtained for the single
layers.
When a coatings on a substrate is submitted to tensile
tests, the response of both the film and the substrate is
entirely elastic at low strain ( lower than 0.8%). At a
critical longitudinal deformation of the substrate, es ,
xx,c
the coating begins to crack as it is much stiffer than the
substrate. The critical cracking stress attained at coating
failure is denoted sf .
xx,c
The cracking phenomenon can be described in successive stages. At crack onset, the coating will develop a
series of regular and parallel spaced cracks, perpendicular to the loading direction. These initial cracks will
multiply rapidly after the crack onset. With increasing
deformation additional transverse cracks appear progressively and the distance separating two consecutive
cracks decreases. This evolution can be followed by the
crack density parameter D, which is defined as the
number of transverse cracks over a given length.
Continuing the longitudinal strain, this parameter
which grows at the beginning of the deformation will

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E. Harry et al. / Surface and Coatings Technology 125 (2000) 185189

reach a constant value: the crack saturation density,

D , corresponding to a minimal length between two
sat
cracks. The vicinity of the crack-free surfaces lowers the
global stress level in the coating under the critical
cracking stress sf [4]. When saturation of the cracks
xx,c
is reached, if the deformation continues, no new cracks
appear; but the existing ones will continue to open, with
increasing plastic deformation in the substrate, concentrated at the crack tip [4].
The critical strain for the substrate is determined
experimentally [4], and the critical cracking stress of the
coating is deduced by taking into account the residual
stresses pre-existing in the coating, sf . The critical
r
cracking stress can be written as:
sf =Efes +sf .
(2)
xx,c
xx,c
r
Experimental mean values of es and sf are reported
xx,c
xx,c
in Table 1. When considering the existence of defects in
sputtered coatings, resulting from the growth process or
previously existing on the substrates, this cracking stress
may be associated with the presence of singularities preexisting in the coatings. This explains the very low
measured values.
Determination of the fracture toughness of the films,
Kf , depends on the parameters mentioned above. It is
1c
based on the energy balance in the strained system when
the coating cracks. The theoretical approach has been
previously described in detail in the case of single layers
[4,5]. It can be extended to our multilayered coatings
since the elementary layers have the same Youngs
modulus and level of residual stress, and assuming
perfect cohesion at layer interfaces. In fact, SEM observations of the cross-section of the multilayered coatings
do not reveal any delamination or buckling at the
interfaces between the tungsten and W(C ) layers when
the films are uniaxially strained. Therefore, the fracture
toughness of the multilayered coatings can be written
as:

C A B

Ef
sf
tf(sf )2 pF
+ xx,c .
(3)
xx,c
Es
3ss
y
F is a function of the elastic modulus ratio [12], and
ss is the yield strength of the substrate. The mean values
y
of the calculated fracture toughness are given in Table 1.
The low values of the cracking parameters character-

Kf =
1c

ise the brittleness of the multilayered coatings, as

observed for the single layers. However, the multilayered
coatings exhibit critical cracking stress and fracture
toughness larger than those determined for the W(C )
films. The combination of hardness [ W(C ) layers] and
toughness (tungsten layers) in a multilayered structure
appears to improve the failure properties of hard coatings. In the case of the four-layer coatings, the cracking
parameters come close to those of the pure metal films.
In addition, the results given in Table 1 reveal a higher
fracture toughness for the four-layer coatings
4L-W(C )/W (with a total thickness of 14 mm and single
layers 3.5 mm thick) than for the bilayer coatings
2L-W(C )/W#3 (14 mm thick and based on two layers of
7 mm thickness) and 2L-W(C )/W#1 (thickness 7 mm,
with elementary layers 3.5 mm thick). The cracking
behaviour of the coatings appears to depend on the
arrangement of the films (single layers, multilayered
structures), the total thickness of the coatings, and the
thickness of the elementary layers. A judicious choice
of the number and thickness of the single layers in
multilayered structures should optimise the in-service
performance of the coatings for a given application.
The experimental evolution of the transverse crack
density (D) of the multilayered coatings is plotted against
the applied strain in the substrate (es ) in Fig. 1. The
xx,c
following empirical relation, based on a Weibull-type

Fig. 1. Transverse crack density of the bilayer coatings 2L-W(C )/W #1

(+), #2 ($) and #3 (&), and of the four-layer coatings 4L-W(C )/W
(%), versus longitudinal strain applied to the substrate.

Table 1
Experimental values of critical strain of the substrate resulting in film cracking, es , critical cracking stress of the coating, sf , the fracture
xx,c
xx,c
toughness, Kf , and the scratch critical load, L , for the bilayer and four-layer coatings
1c
c
Coating
2L-W(C )/W

4L-W(C )/W

#1
#2
#3

Thickness (mm)

es (%)
xx,c

sf (MPa)
xx,c

Kf (MPa m1/2)
1c

L (N )
c

3.5
7
14
14

0.806
0.787
0.7825
0.824

224
148
130
297

0.7
0.6
0.8
1.9

55
65
>100
>100

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E. Harry et al. / Surface and Coatings Technology 125 (2000) 185189

distribution function, was applied to describe the crack

density D as a function of the deformation es [13]:
xx,c
D(es )=D {1exp[A(es es )a]},
(4)
xx
sat
xx
xx,c
where A and a are constant parameters which depend
on the film/substrate system. The exponent a is known
as the Weibull modulus.
The transverse crack density D is obtained from
sat
the experimental plot of D(es ) at saturation (Fig. 1).
xx,c
Notice that A and a are also determined experimentally.
They are respectively the ordinate at zero point and
the slope of the line obtained from the plot of
ln{ln[1(D/D )]} versus ln(es es ). The values
sat
xx
xx,c
of the parameters D , a and A involved in Eq. (4) are
sat
reported in Table 2.
The values of the Weibull modulus range from 0.517
to 0.682 for the bilayer coatings layers, depending on
the coating thickness; and appear to be much higher for
the four-layer coatings, of the order of 0.873. We may
recall that the Weibull modulus expresses the statistical
scatter of events: a high Weibull modulus indicates a
low scatter [11]. The Weibull analysis gives a mathematical tool for predicting the fracture probability of a
structure. In our case, the Weibull modulus appears to
be small, reflecting a high probability of cracking of the
coating and then the presence of numerous defects. As
a comparison, soda-lime glass has a Weibull modulus
of 23 and polysilicon films have a value of 711 [11].
The Weibull modulus tells nothing about the severity of
the defects or their location. However, the difference in
Weibull modulus obtained for the multilayered coatings
may indicate the existence of different types and/or
densities of defects. In our case, a larger number of
interfaces does not seem to generate a higher defect
density or increase the fracture probability of the films,
since the parameters characterising the cracking resistance of the films (sf , Kf , a) are found to be higher
xx,c 1c
for the four-layer coatings than for the bilayer coatings.
The cracking behaviour of multilayered coatings has
been little investigated. In particular, the work of Marieb
et al. [14] on coatings composed of a tungsten layer
deposited on a titanium nitride layer which is deposited
on aluminium substrates, shows that the transverse
crack density of the multilayered coatings is similar to
that obtained for a single layer of titanium nitride. This
suggests that the mechanical behaviour of the multilayTable 2
Experimental values of the saturation crack density, D , the Weibull
sat
modulus, a, and the constant, A, for the multilayered coatings
Coating
2L-W(C )/W

4L-W(C )/W

#1
#2
#3

D (cracks mm1)
sat

50.6
37.3
20.8
22

0.682
0.576
0.517
0.873

0.599
0.434
0.606
0.256

ered coatings is controlled by the layer at the interface

between the film and the substrate. For our
film/substrate systems, this does not seem to be verified.
In fact, for the bilayer coatings, we noted that at
saturation the corresponding crack densities D
sat
decreased from 50.6 to 20.8 when the coating thickness
increases from 3.5 mm to 14 mm, showing a larger
average intercrack spacing for thicker films. This dependence can be described by an empirical equation, written
as:
B
D =
.
sat (tf)n

(5)

The parameters B and n obtained from the experiments

are 110.3 and 0.63, respectively, for the bilayer coatings
on the stainless steel substrates; they were found to be
43.9 and 0.33, respectively, for tungsten single layers on
stainless steel substrate [5]. The empirical model for the
bilayer coatings, describing the evolution of the saturation crack density as a function of coating thickness,
differs from that obtained for the tungsten elementary
layers. This result indicates that the cracking behaviour
of the multilayered coatings is not affected only by the
nature and thickness of the interfacial layer. This is
supported by the value of D obtained for the foursat
layer coatings (22 cracks mm1), which appears to be
different from that of the tungsten layer of 3.5 mm
thickness (50.6 cracks mm1).
The results show that the cracking properties of
multilayered coatings depend mainly on the total thickness of the films and the arrangement of the elementary
layers (number of layers, thickness of single layers, layer
interactions).
When increasing the substrate strain to 25%, no
debonding of the film is observed at layer interfaces and
at the substrate/coating interface. This reveals that the
adhesion between the film and the substrate is good,
but cannot be characterised through tensile tests.
Therefore, scratch experiments were performed on these
coatings.

5. Adhesion characterisation
The objectives of performing scratch tests are to
evaluate the adhesion of the coatings to the substrate
and then to rank the coatings with respect to debonding
resistance. This investigation was based on determination of the critical scratch load values, L , characterising
c
the decohesion between the film and the substrate.
Acoustic emission measurements allow detection of this
load, corresponding to delamination of the coatings
observed by optical examinations of the scratches and
saturation of the acoustic burst.
The experimental values of the critical scratch load

E. Harry et al. / Surface and Coatings Technology 125 (2000) 185189

L are reported in Table 1. For the bilayer coatings

c
2L-W(C )/W#1 and 2L-W(C )/W#2, decohesion of the
films from the substrates is found to occur at the loads
50 N and 62 N, respectively. As for the bilayer coating
2L-W(C )/W#3 and the four-layer coatings 4L-W(C )/W
of 14 mm thickness, the critical scratch loads could not
be determined since saturation of the acoustic burst was
not reached under a load range of 0100 N. The critical
scratch load was found to be higher than 100 N. Our
multilayered coatings appear to adhere very well to
stainless steel substrates, according to the very high
value of L . Indeed, a maximum adhesion can be reached
c
for the thickest films. These results emphasise the effect
of film thickness on the mechanical behaviour of the
multilayered coatings.
Examinations of the cross-section of the scratches by
SEM show that multilayered coatings are subjected to
detachment at layer interfaces [6 ]. The remaining parts
of the film still protect the substrate surface against
interactions with the environment until complete
removal of the coating. However, the progressive delamination of the multilayered coatings may result in a
reduction of their reliability, which can affect the
in-service performance of the coating/substrate system.
Thus, graded coatings might appear to be more suitable
candidates for protective coatings [6,15].

6. Conclusion
In situ microtensile tests were performed on systems
consisting of multilayered coatings deposited by magnetron sputtering on stainless steel substrates. The multilayered coatings were based on the stacking arrangement
of two or four tungsten and tungstencarbon [ W(C )]
single layers. The rupture properties of the films were
characterised by specific parameters, such as the critical
cracking stress and the fracture toughness deduced from
an analytical model, and by the evolution of transverse
crack density with respect to applied strain. The cracking
probability was analysed through a Weibull analysis.
The calculated values of the Weibull modulus revealed
a high probability of cracking, supported by the low
measured values of the fracture toughness and the

189

existence of defects in the films. The analysis showed a

significant effect of the number and thickness of the
elementary layers on the fracture resistance of the multilayered coatings. Indeed, the coatings based on four
thin layers exhibited the highest fracture toughness and
Weibull modulus.
The adhesion of the coatings on substrates was
characterised through scratch experiments. Our multilayered coatings appeared to adhere well on stainless
steel substrates, and no delamination was observed and
detected for the thickest films. However, delamination
at layer interfaces could be observed, resulting in a
reduction in the reliability of the films, before complete
decohesion.

References
[1] A. Cavaleiro, M.T. Veira, Mater. Sci. Eng. A 140 (1991) 631.
[2] P. Monge Cadet, F. Pellerin, G. Farges, D. Rickerby, E. Quesnel,
Propulsion and Energetics Panel SymposiumAGARD Conference
Proceedings No. 558, Rotterdam vol. 31 (1994) 1.
[3] D. Garg, P. Ndyer, D.B. Dimos, S. Sunder, J. Am. Ceram. Soc.
75 (4) (1992) 1008.
[4] E. Harry, A. Rouzaud, M. Ignat, P. Juliet, Thin Solid Films 332
(12) (1998) 195201.
[5] E. Harry, M. Ignat, A. Rouzaud, P. Juliet, Surf. Coat. Technol.
111 (23) (1999) 177183.
[6 ] E. Harry, A. Rouzaud, P. Juliet, Y. Pauleau, Thin Solid Films
342 (12) (1999) 208214.
[7] A. Rouzaud, E. Barbier, J. Ernoult, E. Quesnel, Thin Solid Films
270 (1995) 270.
[8] M. Ignat, Key Eng. Mater. 116117 (1996) 279.
[9] M.F. Asbhy, D.R.H. Jones, Materiaux vol. 1 Dunod, Paris, 1991..
[10] C.E. Kalmas, J.F. Mansfield, G.S. Was, J.W. Jones, J. Vac. Sci.
Technol. A 12 (3) (1994) 883.
[11] S. Greek, F. Ericson, S. Johansson, J.-A. Schweitz, Thin Solid
Films 292 (1997) 247.
[12] M.S. Hu, A.G. Evans, Acta Metall. 37 (3) (1989) 917.
[13] A. Mezin, J.-P. Chambard, J. Lepage, M. Nivoit, Thin Solid Films
185 (1990) 57.
[14] T. Marieb, M. Ignat, H. Fujimoto, P. Flinn, in: A.S. OatesW.F.
Filter, R. Rosenberg, A. Lindsay Greer, K. Gadepally (Eds.),
Thin Films: Stresses and Mechanical Properties, Mater. Res. Soc.
Symp. Proc. vol. 391, Materials Research Society, Pittsburgh, PA,
1995, p. 85.
[15] Y. Gachon, Etude de lerosion par des particules solides de revetements multicouches obtenus par procede PVD sur substrat metallique (base titane). Thesis, Ecole Centrale de Lyon, France, 1997.