Journal of Solid Mechanics Vol. 3, No.

2, 2009

and Materials
Engineering
New Measurement Method for Adhesion of
Hard Coating Film*
Kaoru IKENAGA**, Akira YANAGIDA** and Akira AZUSHIMA**
** Graduate school of Engineering
Yokohama National University
79-5 Tokiwadai, Hodogaya-ku, Yokohama, Japan
E-mail:k-ikenaga@ndkinc.co.jp

Abstract
Various surface coating technologies have been applied to improve the tribological
and mechanical properties of thin films. For the use of surface modified tools and
parts under severe conditions, thin films with high adhesion strength are required.
To quantitatively measure the adhesion of coating films on substrates a new method
for the measurement of hard coating film was developed which consists of an
indentation and an AE (Acoustic Emission) system. TiN coatings were deposited
onto substrates using arc ion plating PVD. Indentation tests were conducted on
substrates with different film thicknesses of 3, 5, and 7 µm. Two specific loads,
denoted the “Critical load”, and the “Fracture load” were defined. The critical load
and fracture load correlate to the initiation of delamination and film fracture. The
critical load was calculated a finite element calculation and SEM observation.

Keywords: PVD, AE(Acoustic Emission), Adhesion, Critical Load , Fracture Load

*Received 25 Aug., 2008 (No. 08-0599)
[DOI: 10.1299/jmmp.3.347]
1. Introduction
Recently, hard coatings produced by the vapor deposition process have become widely
used in industrial components. These coatings are sought after as their properties can be
tailored for each specific application. As adhesion between the coating and the substrate is
an important property, a quantitative measurement method for the adhesion of hard coating
films is needed.
A scratch test is used to evaluate the adhesion of hard coating films [1,2] as well as their
tribological properties. However, the relationship between the critical load in the scratch test
and the adhesion strength is not quantitatively obvious. This is because the critical load of
the scratch test is influenced by many factors such as substrate hardness, film roughness and
surface thickness. Kagawa et al. proposed a method for the evaluation of fracture strength
of thin films by means of indentation with a spherical indenter, and the usefulness of that
method was investigated [3,4]. These fracture initiation loads were determined using AE
(acoustic emission) analysis equipment [3,4]. The AE system was also tested by a
nano/micro indentation test for the detection of radial cracks, and lateral cracks in columnar
grains of TiN films on silicon [5] and other film/substrate systems [6-8]. The fracture mode
of the coating changes as the film thickness to indenter radius ratio changes [9]. For the
nano-indentation test, a circular crack is initiated close to contact edge and propagates
during indentation. Delamination occurs during unloading. It is thus difficult to evaluate
adhesion strength by the nano-indentation test. A large indenter is usually selected because
it approximates contact conditions in practice and it is expected to change the fracture mode

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because of the low ratio of film thickness to indenter radius.

The sensitivity of the AE sensor was then increased, to detect the fracture, and the
interfacial delamination of thin films. However, the relationship between the detected AE
signal before crack initiation and fracture events in the specimen was not clear.
Elastic-plastic finite element analysis was also conducted to correlate the AE signal detected
during indentation load to the initiation of thin film delamination on the substrate.

2. Experimental conditions
2.1 Specimens
TiN coatings were deposited using an arc ion plating PVD apparatus (AIP3012
KOBELCO). A titanium cathode was used for the deposition of TiN coatings. A WC-Co
block was used as a substrate. Specimens had dimensions of 10 mm× 10 mm× 13 mm,
and the hardness was controlled to 1600 HV by heat treatment. Each substrate was finished
to a constant surface roughness of 0.02 µmRa. Before insertion into the chamber substrates
were cleaned ultrasonically in an isopropanol bath. Before deposition the substrate was
gradually heated to 327K and the chamber was evacuated to 1.3× 10-3 Pa simultaneously
to avoid contamination. The substrate surface was then sputtered and cleaned Ar for 0.9 ks
at a pressure of 1.33 Pa and a substrate bias voltage of -400V. Nitrogen gas was introduced
into the deposition chamber through a gas control system. Coating conditions are
summarized in Table 1. TiN coatings were deposited for 0.3 Ks-2.1 Ks under a nitrogen gas
pressure of 1.33 Pa at an arc current of 150 A. The substrate bias voltage was controlled to
-50V. TiN coating thickness was controlled to be 3, 5, or 7µm.

Table.1 Coating conditions

Bias voltage (V) -50
Arc current (A) 150
Reactive gas pressure (Pa) 1.33
Deposition time (ks) 0.3～2.1

2.2 Measurement apparatus and experimental conditions

A schematic representation of the measurement apparatus is shown in Fig. 1. The
apparatus consists of a SERVOPULSER (EHF-FB5KN-10LA, SIMADZU) and an AE
system (MISTRAS-2001, PHYSICAL ACOUSTICS CORP.). Two types of AE resonant
frequency of 300, 500 kHz and 45 dB gain are used. An adhesion of TiN films is evaluated
using the indention method. Tests are performed using a WC-Co sphere indenter with a
diameter of 6 mm and are done by continuously increasing the load up to 3.5 kN at a
loading rate of 10 N/s. The aim of this test is to determine the load at which initial
delamination occurs and the load at which the TiN films fail. During these tests acoustic
emissions are recorded. Two AE sensors are mounted directly on the sides of the specimen.
The conditions used for the AE system are summarized in Table 2. During the indentation
test the energy, the number and the dB of the acoustic emission signals are recorded
digitally. The AE energy from the data was used for evaluation. The AE energy is
determined as the integration of the number and the dB of the acoustic emission signal.
Acoustic emission signals are relative to fractural events due to the delamination of the
interface, film cracks and substrate cracks. Experimental results of acoustic emission vs.
time during the indentation are shown in Fig. 2. Two specific signals are observed in Fig. 2
and the first signal is referred to as the ‘Critical Load”. After AE the signal reaches a peak
value and no or a small AE signal is detected. A second rising signal is then detected and is
referred to as the “Fracture load” because a surface crack is observed by SEM around its
load (details are described further on).

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To compare indentation tests SEM observations of indentation impressions are conducted

with every 0.2 kN load. The acoustic event that correlates to fracture development in the
specimen is discussed in the following section.
The crystallographic structure of these coatings was investigated by XRD (MO3XFH,
MAC Science) using CuKα radiation with an energy of 40 KeV (tube voltage 40 KV, tube
current 4 mA). The degree of preferred orientation was estimated from XRD peak intensity.
The film thickness of the deposited TiN coating was measured using a stylus profile meter
(Surfcom 590A TOKYO SEIMITU). A CSEM Revetest scratch test instrument was used to
characterize the adhesive strength of the substrate deposited TiN films. Vickers hardness
measurements were performed using a micro-Vickers hardness tester under a load of 98 mN
for 15 s. After these tests TiN coating surface impressions were investigated using a
scanning electron microscope (SEM JSM5310, JEOL).

Table 2. Setup conditions for the AE system

FIXED
Threshold
45 dB

Pre-Amp (dB) 40

Filter Low ( kHz) 100

Filter High ( kHz) 2000

AE sensor
(500kHz)
Part of Indentation
Indenter

AE sensor
(300kHz)

Specimen
SERVOPULSER

Fig.1. A schematic representation of the measurement apparatus

10N / s
Load / N

Critical load Fracture

Ｓｅｃｏｎｄ load
ｓｉｇｎａｌ 5μm
AE energy

Ｆｉｒｓｔ ｓｉｇｎａｌ

Ｔｉｍｅ / s

Ｔｉｍｅ (sec)
Fig. 2. AE signals from indentation tests

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3. Results and discussion

3.1 Materials and mechanical proportions of the TiN coating

Figure 3 shows the XRD pattern of the TiN coated specimen with a thickness of 5 µm and
at a substrate bias voltage of -50 V with 2θ scanning from 30° to 50°. At a bias voltage of
-50 V a strong (200) orientation is observed. The results for film thicknesses of 3 and 7 µm
were similar to that for 5 µm. The intensity of (111) slightly increases as film thickness
increases. Figure 4 shows the micro-Vickers hardness of the deposited TiN coatings with
film thicknesses of 3, 5 and 7 µm. The micro-Vickers hardness generally increases with
increasing film thickness. Figure 5 shows the critical scratch loads as measured by the
scratch test instrument. The critical scratch load was confirmed by optical microscopy at the
onset of coating failure. The critical load increases with increasing film thickness and the
value at 5 µm is about 70 kN.

7.0μm TiN(200)

10000 TiN(111)
Intensity (counts)

5.0μm TiN(200)

10000
TiN(111)

3.0μm
TiN(200)
10000 TiN(111)

0
30° 35° 40° 45° 50°
2θ
Fig. 3. X-Ray diffraction patterns of TiN coatings

3000
/ Hv

2750
Vickers hardnessHv

2500
MicroＭｉｃｒｏｈａｒｄｎｅｓｓ　/

2250

2000

1750

1500 Vickers
Vickers hardness
hardness
Load
load 98mN
98mN
1250

1000
0 1 2 3 4 5 6 7 8
Film thickness / μｍ
Film thickness / μm

Fig. 4. Micro-Vickers hardness of the deposited TiN Coatings of different thickness.

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100

oad //NN
LLoad
50
Critical load
Critical Load
( scratch test)

0
0 1 2 3 4 5 6 7 8
F ilm th ic kn e ss / μ ｍ
Film thickness / μm

Fig. 5. Critical scratch loads measured by the scratch test

3.2 Critical load of TiN coatings

3.2.1 Reliability of measured values

To evaluate the reliability of the measured values for the critical load, experiments were
carried out eight times at a loading rate of 10 N/s using a 5 µm specimens. Figure 6 shows
the eight measured values of the critical load. The average critical load value for the film
with thickness of 5 µm is 0.99 kN. From experimental results it is thus understood that the
reliability is high. And the average critical loads for the film thicknesses of 3 µm and 7 µm
are 0.75 kN and 1.20 kN, respectively.

1.5
1.5

Ave. 1.2kN
Load/ /kN

1.0
1.0
kN

Ave. 0.99kN
Load

Ave. 0.75kN

0.5
0.5 Critical load(Indent)
7μm

Average (0.99kN)
5μm
3μm

00
1
1 22 33 44 55 6 6 7
7 88 9 10
Sample number
Sample number

Fig. 6. Dispersion of the critical load under the same experimental conditions.

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3.2.2 Effect of the film thickness on the critical load

Figure 7 shows the relationship between the critical load and film thickness. The critical
load increases as coating thickness increases.

2.0

Ｃｒｉｔｉｃａｌ　ＡＥ　Ｌｏａｄ　/kN
Critical AE Load / kN
1.5

1.0

0.5
Average
Critical AEvalue
load of
critical AE load
0.0
0 1 2 3 4 5 6 7 8
Film
Filmthickness / μｍ
thickness / μm
Fig. 7. The relationship between the critical load and the film thickness

3.3 Fracture load of TiN coatings

3.3.1 Effect of film thickness

Figure 8 shows the relationship between the load detected from AE signal (fracture load)
and the film thickness. The fracture load generally increases as the film thickness
increases. The dependence on film thickness is found to be smaller compared with the
effect of the critical load on the film thickness. It is likely that the difference in measured
values for the coating with a thickness of 5 µm was a measurement error because circular
crack detection by SEM was very difficult.

4.0
3.8
3.6
3.4
kN
Load // kN

3.2
3.0
Load

2.8
2.6 Observed crack
Obsevation load load
of crack / kN / kN
2.4
2.2 AE flacture
Load Load
detected at /
AEkN
signal / kN
(Fracture load)
2.0
0 1 2 3 4 5 6 7 8
Film thickness / μｍ
Film thickness / μm
Fig. 8. Comparison of the observed crack load and the load detected
from the AE signal (fracture load) for each film thickness.

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3.3.2 SEM of the coating surface

Circular cracks on TiN coating specimens with film thicknesses of 3, 5 and 7 µm were
detected by SEM. Surface photographs of the TiN coating specimens, from the indentation
test in which fracture cracks were detected, are shown in Figures 9 (a), (b) and (c).
The loads in Figs 9 (a), (b) and (c) were 3.0, 3.2 and 3.4 kN, respectively. These values
are also shown in Fig. 8. The loads at which fracture cracks were observed on the coated
surface is in good agreement with the fracture load detect by AE analysis as shown in Fig.
8. Values from the AE analysis are slightly less, indicating that fracture load detects the
initiation of circular cracks and thus it is expected that the crack initiates at the interface.

Ｃｒａｃｋ Ｃｒａｃｋ

10µm
10µm
3.0ｋＮ 3.2ｋＮ

(a) Film thickness 3.0 µm (b)Film thickness 5.0 µm

Ｃｒａｃｋ

10µm

3.4ｋＮ

(c) Film thickness 7.0 µm

Fig. 9. Observation of cracks in the TiN coating by SEM

3.4 Finite element analysis

3.4.1 Finite element model

Elastic-plastic finite element analysis was conducted under approximate axisymmetric
conditions. This code was developed by Yanagimoto et al., and was based on a
co-rotational formulation. We modified the code to apply a contact problem and account
for the elastic-plastic deformation of the sphere indenter. A contact constraint condition
was satisfied by Lagrange-Multiplier Method. The yielding equation of the substrate was
taken from the experimental results of Milman et al. Material parameters used for this
analysis are shown in Table 3. The part of the thin film near the interface was divided into
1 µm meshes in thickness direction. However, a slight difference of hardness was found
for each film thickness and the same yield stress was applied to these. We assumed that the
film-substrate interface was perfectly bonded and that the film-indenter interface was
frictionless. The residual stress of the thin film was not considered. The indenter was

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modeled as a hemisphere and a constant velocity was applied to its upper surface indenter
instead of the 10 N/s loading rate as in the experiment. This was done because the
dependence of strain rate on yield stress was not considered. The finite element model
geometry and mesh is shown in Fig. 10.

Table 3 Material parameters used in the analysis

Coating Indentor Substrate

TiN WC-Co WC-Co
Young’s modulus 240 540 620
(GPa)
Poisson’s ratio 0.20 0.22 0.22
Yielding stress(GPa) - 40(0.0025 + ε p ) 0.45
6.5
Y=2.7GPa

Constant velocity

Indenter

Coating

Substrate

Fig. 10. The Finite element model geometry and mesh

3.4.2 Results for and discussion of FE analysis

To investigate the stress condition at the interface the difference in radial stress at the
film-substrate through the z direction is defined as follows:

σ ri +1 − σ ri −1
∆σ ri = (1)
z 2
σ ri is the radial stress at the interface and superscript i denotes the i-th node from the r axis,
σ ri +1 and σ ri −1 are radial stresses for adjacent nodes in the z direction at the film and the
substrate, respectively.
Figure 11 shows the distribution of radial stress and ∆σ ri at indentation critical loads
z
(Fig. 7) for each film thickness.
The contact boundary is also indicated in Fig. 11. The peak stress is located at the
out-of-contact boundary. Figure 12 shows the radial stress peak and ∆σ ri as a function of
z
applied load. The radial stress difference at the indent critical load (0.75, 0.99 and 1.25 kN
for 3, 5 and 7 µm, respectively) coincides with the film thickness at -350 MPa. The critical
load can thus be related to the critical shear stress of 350 MPa at the interface of the film
and the substrate.

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Contact boundary
2000
1000 1500
0
-1000 σr 1000

σr / MPa
3µm

∆σr z / MPa
-2000 5µm
7µm 500
-3000
-4000 ∆σr z
0
-5000 3µm
5µm
-6000 7µm
-500
0.0 0.1 0.2 0.3 0.4 0.5
r / mm

Fig. 11. Distribution of radial stress σr and the difference of radial stress along the Z
direction through the film-substrate interface at indentation critical loads

100
1500 3 µm
5 µm
σr 0
7 µm
Radial stress σr /MPa

-100
1000

/ MPa
-200

-300

z
∆σr
500 -400

-500
∆σr z
0 -600
0.0 0.2 0.4 0.6 0.8 1.0 1.2
Load /kN

Fig. 12. Radial stress peak and the stress difference as a function of applied load

Figure 13 shows the radial stress peak at the film surface and the average radial stress in
the film during loading until the appearance of a crack. Radial stress peaks at the surface
increase as film thickness increases while the average radial stress reduces. The surface
radial stress increases as film thickness increases due to increase of bending stress. As is
shown Fig. 12, the radial stress at the interface increases as film thickness decreases as well
as the gradient of stress, in the same load condition. The change of radial stress through film
thickness becomes larger as film thickness increases. These differences of radial stress are
mainly caused by the difference of Young’s modulus between the film and the substrate.
The effect of Young’s modulus increases as the film thickness increases. Then the difference
between the surface radial stress and the average radial stress increases as increases the film

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thickness. The radial stress peak at the crack initiation load is different for each film
thickness. The average stress decreases as film thickness increases at the same applied load,
which indicates that the calculated average radial stress of around 1.7 GPa represents the
fracture stress of the thin film qualitatively. The increase of critical load with film thickness
correlates to a decrease in average stress of the films on the substrate. For a more accurate
discussion about fracture strength the boundary conditions of the interface after
delamination and residual stress must be considered.

2000
Radial stress σr /MPa

1500

1000
Surface Average
3 µm 3 µm
500
5 µm 5 µm
7 µm 7 µm
0
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5
Load /kN

Fig. 13. Changes in radial stress peaks at film surfaces and the average radial stress
in films

4. Conclusion

The adhesion strength of coatings was investigated by indentation using a newly

developed adhesion measurement device and the following results were obtained:

(1) Data obtained from the AE signal in this study were consistent for every coating
thickness. Acoustic emission analysis enables the predication of initiation behavior for
film-substrate interface and for the fractures of films on substrates.

(2) The gradient of the radial stress peak of the interface as calculated by FE analysis is
equivalent for each film thickness, at the indentation load, and this result indicates that the
critical load can relate to the critical shear stress at the interface of film and substrate.

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