Fragmentation Test Method for Adhesion Analysis of Coatings In Situ in a Microscope

Y. Leterrier
Laboratoire de Technologie des Composites et Polymres (LTC)
Ecole Polytechnique Fdrale de Lausanne (EPFL)
CH-1015 Lausanne, Switzerland
Introduction
Mechanical integrity is a key attribute of coatings, which should not crack and delaminate
during processing and during service life. Numerous methods are available to determine the
adhesion of coatings, including tape and pull-out tests, and indentation and scratch
techniques. The accuracy of these methods is however compromised by the presence of third
body interactions, such as indenter-coating friction in case of scratch and indentation tests, or
adherent-coating traction in case of peel and pull-out tests. The fragmentation test method
detailed in the present note is free of third-body interactions. It enables quantifying the
cohesive properties (which control cracking) and the adhesive properties (which control
delamination) of coatings on high-elongation substrates. The method has been used to analyze
a broad range of coating/substrate combinations, including inorganic coatings on polymers [13] and steel (e.g., [4]), and organic coatings on polymers (e.g., [5]). The following Section
introduces the theory of coating fragmentation and calculation of the adhesive strength. The
experimental conditions are detailed in a further section. Finally two application examples are
given to illustrate the method, with focus on adhesive strength of an organic coating on a PET
substrate, and a transparent electrode on a PEN substrate.
Theory
In a fragmentation test, a coated substrate is loaded under uniaxial tension, and the damage
state in the coating is analyzed as a function of strain. The test is applicable in case of high
elongation substrates. Upon straining, coating cracks form due to interfacial stress transfer
between the substrate and the coating. With increasing strain the number of cracks increases
steadily with increasing strain until it reaches a saturation value. This fragmentation process
reveals 3 stages of damage as shown in Figure 1.
Stage I: crack onset and random cracking. Cracks initiate in the coating at defect sites and
start propagating perpendicular to the loading direction. The interaction between cracks is
negligible and the generation of new cracks is governed by the statistical distribution of
defects within the coating. The fragmentation test allows us to measure directly the critical
strain crit (also termed crack onset strain, COS) at which cracks start to form in the coating.
Stage II: mid-point cracking. The size of coating fragments approaches the critical length for
stress transfer. The generation of new cracks diminishes and transverse buckling is observed
across fragments due to Poissons ratio effects.
Stage III: delamination and saturation. No further cracks are generated in this stage and the
density of cracks reaches a saturation value, CDsat. Delamination becomes the dominant
failure mechanism.

II

III

Crack density

CDsat

crit

Strain

Figure 1. The three stages of fragmentation of a coating under uniaxial loading: at a critical strain (crit) the
sample starts cracking (stage I), at higher strain mid-point cracking begins and transverse fragment buckling
initiates (stage II) and above a certain strain, the crack density becomes constant, no more cracks are formed and
the crack density at saturation (CDsat) is reached (stage III).

The application of the theory of stress transfer allows the calculation of the interfacial shear
strength (IFSS), which characterizes the practical adhesion of the coating layer in the
mechanical sense, from the measured critical strain crit and crack density at saturation, CDsat:

IFSS = 1.337 hc Ec crit CDsat

(1)

where hc and Ec represent the coating thickness and elastic modulus, respectively.
Experimental
Two coated substrates were used. The first was a 75 m thick polyethylene terephthalate
(PET) film coated with a 3.5 m thick organic coating. The elastic modulus of the coating
was equal to 5 GPa. The second was a 50 m thick polyethylene naphthalate (PEN) film
coated with a 100 nm thick transparent conducting oxide (TCO) coating. The elastic modulus
of the TCO coating was equal to 120 GPa. Such films are common in food packaging and
flexible electronic devices.
The application of a tensile load to rectangular film specimens (typical gauge dimensions
5 mm x 20 mm) was achieved with the TST350 stage mounted under an optical microscope
(Olympus BX60). This setup enables analyzing coatings of thickness down to 50 nm, below
which a scanning electron microscope becomes necessary [6]. Cracking of the coatings was
analyzed at increasing strain levels in terms of crack density (CD), calculated from the
average of the number of cracks, Ni, counted on k micrographs of width W, at strain , as
k
CD = (1+ ) N i / kW . The factor (1+) corrected for crack opening to a first
i=1
approximation.
Results
Figure 2 shows the progressive tensile damage in the organic coating during loading the
polymer substrate. The coating was intact before loading (Fig. 2a). Initial cracks were
detected around 4% strain (Fig. 2b). Upon further straining the crack density increased rapidly

(Fig. 2c) until saturation, with some evidence of buckling delamination at the edges of coating
fragments (Fig. 2d). The fragmentation process is depicted in Figure 3. The critical strain and
crack density at saturation were found to be equal to 3.5% and 28 mm-1, respectively. The
IFSS between the organic coating and the polyester substrate was calculated using Equation 1
and the experimental data, and found to be equal to 21 MPa.

(a; 0%)

(b; 3.9%)

(c; 6.6%)

(d; 19.2%)

Figure 2. Optical micrographs of tensile damage in the organic coating during loading the PET substrate. The
strain levels are indicated below each micrograph.

Figure 3. Fragmentation of a 4 m thick organic coating on a PET substrate under uniaxial loading.

Figure 4 shows the fragmentation process of the ultrathin TCO coating on the PEN substrate.
The initiation of tensile damage in the form of cracks of finite length is evident. Saturation
occurred around 10% strain. The damage state at very high strain combines a high density of
tensile cracks and transverse buckling features. The critical strain and crack density at
saturation were found to be equal to 1.5% and 155 mm-1, respectively. The IFSS between the
TCO coating and the PEN substrate was calculated using Equation 1 and the fragmentation
data, and found to be equal to 37 MPa.
The method also enables one to obtain the critical radius of curvature for coating cracking,
which is relevant for flexible electronic devices. The critical radius is equal to the total film
thickness (50.1 m) divided by twice the critical strain (2 x 0.015). In the present case this
critical radius was equal to 1.7 mm.

Figure 4. Fragmentation of a 100 nm thick transparent conducting oxide film on a PEN substrate under uniaxial
loading. The micrographs were taken with a green filter to emphasize contrast and show crack initiation and
crack saturation, with extensive buckling.

Conclusions
The fragmentation test method is a tensile test carried out in situ in a microscope to measure
the strain at failure and the adhesive strength of coatings on high-elongation substrates. The
key advantage of the method is that it is free of third-body interactions (such as indenter
friction in case of scratch test). Other benefits of the in-situ method include the direct
observation of damage processes such as crack initiation and delamination. Its accuracy relies
on the measurement of the density of tensile cracks in the coating vs. strain. The combination
of the optical microscope (with sufficient contrast to resolve damage in coatings thicker than
50 nm) with the compact and accurate TST350 stage was found to be optimal to reach the
performance level required for the fragmentation method.
References
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Lausanne, December 2009