Materials Science and Engineering A354 (2003) 140
/145

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Effect of peak load on the determination of hardness and Young’s

modulus of hot-pressed Si3N4 by nanoindentation
Jianghong Gong *, Hezhuo Miao, Zhijian Peng, Longhao Qi
Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, PR China

Received 5 August 2002; received in revised form 6 December 2002

Abstract

The indentation load
/displacement curves of a hot-pressed silicon nitride were measured under different peak load levels. The
unloading segments of these curves were analyzed using the widely adopted Oliver
/Pharr method. It was found that both the
hardness, H , and the Young’s modulus, E , exhibit significant peak-load-dependence. Empirical approaches were then proposed to
determine the load-independent hardness and modulus. The hardness and modulus deduced from these empirical approaches were
proven to be comparable with the literature reported data measured with conventional methods.
# 2003 Elsevier Science B.V. All rights reserved.

Keywords: Nano-indentation; Hardness; Young’s modulus; Silicon nitride; Ceramics

1. Introduction where hmax is the displacement measured at peak load

During the past several decades, nanoindentation
techniques have been developed [1
/4] and widely used
to determine various mechanical properties, such as
hardness, modulus [5,6] and the properties of thin films
and coatings [7,8]. Most of the previous studies con-
cerning the determination of hardness and modulus
were based on the analysis of the indentation load
/
displacement curves resulting from the nanoindentation
test with the method developed by Oliver and Pharr [2].
In general, the hardness, H, is defined as the ratio of the
peak load, Pmax, to the project area of the indentation
impression, Ac, i.e.
Pmax Pmax
H  ;
Ac 24:5h2c
where hc is contact depth at the peak load. According to
the analysis of Oliver and Pharr [2], hc can be
determined with the following equation
Pmax
hc hmax 0:75 ; (2)
S tests, however, only one or two peak load levels were
* Corresponding author. Fax: /86-10-62771160.
E-mail address: gong@mse.tsinghua.edu.cn (J. Gong).
0921-5093/03/$ - see front matter # 2003 Elsevier Science B.V. All rights reserved.
doi:10.1016/S0921-5093(02)00940-1
and the second term in the right-hand side of the
equation represents the displacement of the specimen
surface at the perimeter of the contact at peak load. S
( /dP /dh ) is the initial unloading stiffness, i.e. the slope
of the unloading segment of the experimentally recorded
load
/displacement curve at the peak load. To determine
S , Oliver and Pharr [2] proposed following empirical
expression to describe the unloading portion of the
load
/displacement curve,
P a(hhf )m ; (3)
where P is the indentation load, h is the indenter
displacement, a and m are empirically determined
fitting parameters, and hf is the final displacement after
(1) complete unloading and also determined by curve
fitting. Once the parameters a , m and hf are obtained
by curve fitting, the initial unloading stiffness, S , can be
established by differentiating Eq. (3) at the maximum
depth of penetration, h/hmax.
Nanoindentation tests have been conducted on sev-
eral types of ceramics [2,3,6,9
/11]. In most of these
used for the determination of hardness and modulus
from the analysis of the load
/displacement curves. In
fact, analyses [1
/4] aiming at extracting hardness and
modulus from the load
/displacement curves usually
 J. Gong et al. / Materials Science and Engineering A354 (2003) 140
/145
assumed that the hardness can be treated as a constant,
although several authors [12,13] have pointed out that
there may be an indentation size effect (ISE) in the
nanohardness, i.e. the nanohardness may vary with the
peak load.
In order to gain a basic knowledge of the ISE in the
nanohardness of brittle ceramics, nanoindentation tests
were performed on a hot-pressed silicon nitride at
different peak load levels and the resultant load
/
displacement curves were analyzed using Oliver
/Pharr
method. Then the effect of peak load on the determina-
tion of hardness and Young’s modulus was examined.
2. Experimental
Commercial hot-pressed silicon nitride (FD-05,
Found Corp., China) was selected as the test material.
According to the information provided by the supplier,
the test material has a density of 3.28 g cm 3 and a
microhardness of 16
/18 GPa measured using Vickers
indenter in the load range from 1 to 10 kg.
The test specimen was received with machined sur-
faces. The surface machining damage was removed
mechanically by polishing, ultimately with 0.5 mm
diamond paste, to produce an optical finish.
The nanoindentation tests were conducted with a
Berkovich indenter using a fully calibrated Nano
Indenter XP (Nanoinstruments Innovation Center,
MTS systems, TN, USA). Experiments were performed
using a load
/time sequence like that shown in Fig. 1.
During the test, a personal computer collected and
stored data for the load and displacement as the
indenter was driven into the sample (loading segment)
and then withdrawn from it (unloading segment). The
raw data were then used to construct the load
/
displacement plot. Three indentations were made and,
correspondingly, three load
/displacement curves, each
Fig. 1. The load
/time sequence used in the experimental procedure.
Loading and unloading for each cycle lasted 15 s, respectively, and a
dwell time of 30 s at each peak load was used.
141
containing seven loading/unloading cycles, were ob-
tained.
Some of the resultant indentation impressions were
observed under the atomic force microscopy and typical
AFM image are shown in Fig. 2. As can be seen, no
indentation-induced cracking occurs in the vicinity of
the indentation. In fact, the critical load for Vickers
indentation-induced microcracking for hot-pressed
Si3N4 has been determined to be about 3 N [14,15].
The maximum peak load used in the present study is
only 0.5 N. There is reason to believe that the effect of
microcracking on the determination of hardness and
Young’s modulus by nanoindentation is insignificant.
3. Results
Typical load
/displacement curves obtained in the
present study are shown in Fig. 3. As can be seen, the
unloading and reloading curves are nearly the same.
This suggests that, during the unloading half-cycle, the
deformation in the test material is almost entirely elastic,
implying that the peak load hold period, 30 s, in the
loading sequence is enough to allow the possible time-
dependent plastic effects to diminish.
Studies [16
/18] have suggested that, during the
loading half-cycle in the recording microhardness test,
a linear relationship exists between P /h and h. Similar
phenomenon was also observed in the nanoindentation
test conducted here, see Fig. 4. According to the analysis
of Fröhlich et al. [16], the slope, b, of the P /h/h
straight line may be considered as a measure of the so-
called load-independent hardness, H0, i.e. H0 /kb ,
where k is a constant dependent only on the indenter
geometry and k /1/24.5 for the Berkovich indenter. A
linear regression analysis of the plot shown in Fig. 4
yields b/2.968 mN nm 2 which gives a load-indepen-
Fig. 2. AFM image showing the indentation in the specimens surface.
142 J. Gong et al. / Materials Science and Engineering A354 (2003) 140
/145

unloading cycles have little effect on the loading

portions of the resultant load
/displacement curves.
The unloading segment of each loading/unloading
cycle was analyzed using the Oliver
/Pharr method [2]
and the results are summarized in Table 1.

4. Discussion

4.1. Hardness

Using the best fit-values of the contact depth, hc, the

Fig. 3. Typical load
/displacement curves obtained on the hot-pressed
silicon nitride.
Fig. 4. The experimental data in the loading segments of the load
/
displacement curves shown in Fig. 2 were re-plotted in a P /h versus h
scale.
dent hardness of about 12 GPa. This hardness value is
unacceptably small compared with the microhardness of
the test materials, 16
/18 GPa. Such a small hardness
value can be attributed to the fact that the displacement,
h , used to construct the plot in Fig. 4 is not the real
contact depth. Rather, h is the sum of the real contact
depth and the displacement of the specimen surface at
the perimeter of the contact [2]. However, it should be
noted that the regression analysis returned a correlation
coefficient of 0.999, implying that the repeated loading/
hardness was calculated with Eq. (1) and the results are
plotted as a function of the peak load in Fig. 5. Each of
the data points represents an average of measurements
from three tests and the error bars represent 9/one
standard deviation. Although there was a large scatter in
the hardness determined at lower peak loads, a sig-
nificant indentation size effect was observed, that is, as
the peak load increases, the hardness decreases dis-
tinctly.
The indentation size effect has been examined exten-
sively for the microhardness testing of ceramics [19
/23].
It was suggested that the indentation load, P , and the
resultant indentation size, d , can be correlated with an
empirical equation
P a?0 a?1 d a?2 d 2 ; (4)
where a?0 ; a?1 and a?2 are descriptive parameters derived
from the curve fitting of the experimental results.
Note that the indentation size, d, can be determined
to be proportional to the contact depth at the peak load,
hc, based on the indenter geometry. Thus, an expression
similar to Eq. (4) can be obtained for the nanoindenta-
tion test, i.e.
Pmax  a0 a1 hc a2 h2c ; (5)
where a0, a1 and a2 are constants. Especially, following
the previous analyses [19
/23], the parameter a2 was
considered as a measure of the load-independent hard-

Table 1
Best-fit results for the unloading segments of measured load
/
displacement curves

Pmax (mN) hmax (nm) m S (mN nm 1) hc (nm)

7.9 146.09/9.5 1.689/0.04 0.1789/0.017 112.49/8.9

16.0 215.29/8.2 1.669/0.15 0.2639/0.023 169.39/14.9
31.9 308.59/7.9 1.659/0.07 0.3759/0.018 244.79/7.9
63.3 442.99/8.8 1.659/0.08 0.5289/0.029 352.99/4.9
127.0 638.09/4.5 1.659/0.09 0.7499/0.026 510.79/6.6
253.2 915.49/9.4 1.649/0.03 1.0469/0.036 733.89/4.0
505.9 1298.79/7.4 1.719/0.07 1.5269/0.033 1049.99/9.6
Fig. 5. Variation of the hardness with the peak load.
 J. Gong et al. / Materials Science and Engineering A354 (2003) 140
/145
ness, H0, and both quantities can be related with
H0 ka2 ;
where k is a constant dependent only on the indenter
geometry. For the Berkovich indenter used in the
present study, k /1/24.5.
The application of Eq. (5) to the experimental results
given in Table 1 is now illustrated in Fig. 6. The solid
line in the plot was obtained by a conventional poly-
nomial regression according to Eq. (5). Clearly, Eq. (5)
is proven sufficiently suitable for the representation of
the experimental data. Using the best-fit value of the
parameter a2, 4.3 /104 mN nm 2, the load-indepen-
dent hardness, H0, was calculated with Eq. (6) to be 17.6
GPa, being a reasonable estimation for the hardness of
hot-pressed silicon nitride whose microhardness lies in
the range 16
/18 GPa.
The physical meaning of Eq. (5) has been analyzed
based on both energy balance consideration [20,22] and
proportional specimen resistance (PSR) model [19,21].
Undoubtedly, similar analysis may also be suitable for
the nanoindentation test. In other words, the existing
energy balance consideration and PSR model can be
used to explain the indentation size effect in the
measured nanohardness.
There were several other explanations for the ISE
observed in nanoindentation test, including the surface
pile-up or sinking-in [3,24,25] and the indenter tip
correction [2,26,27]. Analysis [3] has confirmed that,
for brittle ceramics, it is surface sinking-in, rather than
pile-up, that usually occurs during nanoindentation. On
the other hand, the effect of sinking-in on the hardness
determination has been eliminated by using Eq. (2) to
calculate the contact depth. Therefore, there is reason to
believe that surface pile-up or sinking-in is not the main
source of the ISE shown in Fig. 5. The effect of indenter
tip rounding on the hardness determination was ana-
lyzed by several authors and it was suggested that,
considering the existence of a non-perfect indenter tip,
the area term used in hardness calculation, Eq. (1),
Fig. 6. Contact depth, hc, versus the peak load, Pmax.
143
should be revised as
(6) Ac 24:5(hc j)2 : (7)
The constant j is a correction factor for the penetration
depth and defined based on the indenter tip radius.
Substituting Eq. (7) into Eq. (1) and making some
transformation, one would obtain
Pmax  24:5H(j2 2jhc h2c ): (8)
Although Eq. (8) has the same form as Eq. (5), it seems
to be unreasonable to explain the experimental fact
shown in Fig. 6 based only on the indenter tip correction
because the regression analysis of the experimental data
according to Eq. (5) yielded a negative a0-value whereas
Eq. (8) requires a positive a0-value.
4.2. Modulus
It has been suggested that S is an increasing function
of the project area of the elastic contact, A , [2]
dP 2 pffiffiffiffi 2 pffiffiffiffiffiffiffiffiffi
S  pffiffiffi Er A  pffiffiffi Er 24:5hC ; (9)
dh p p
where Er is the reduced modulus defined as
1 1  y2 1  y2I
  ; (10)
Er E EI
where E and y are Young’s modulus and Poisson’s ratio
of the test material and EI and yI are the same
parameters for the indenter.
Eqs. (9) and (10) are the basic equations for the
determination of Young’s modulus by nanoindentation.
Using the experimentally determined S and hc (Table 1),
the Young’s modulus of the hot-pressed Si3N4 examined
was calculated and the results are shown in Fig. 7 as a
function of the peak load. In these calculations, the
Young’s modulus and the Poisson’s ratio of diamond
(indenter) are 1411 GPa and 0.07 [2], respectively, and
the Poisson’s ratio of Si3N4 is assumed to be 0.23 [28].
Fig. 7. The Young’s modulus extracted from the analysis of the load
/
displacement curves as a function of the peak load.
144 J. Gong et al. / Materials Science and Engineering A354 (2003) 140
/145
Clearly, the extracted Young’s modulus exhibits a
strong peak-load-dependence. Therefore, one can con-
clude that the Young’s modulus cannot be extracted
from the load
/displacement curves resulting from only
one peak load.
As can be seen from Eq. (9), there exists a linear
relationship between the initial unloading stiffness, S ,
and the contact depth at peak load, hc, and the reduced
Young’s modulus can be obtained directly from the
slope of the best-fit line. In Fig. 8, the experimentally
determined S is plotted as a function of the contact
depth at peak load, hc. Clearly, a good linear relation-
ship exists between these two quantities. Least-square
regression analysis yielded a slope of 0.0014 mN nm 2
and an intercept in S -axis of 0.021 mN nm 1.
From the slope of the best-fit line, the Young’s
modulus was determined to be 304 GPa. This value
lies in the typical range of the Young’s modulus of
conventional hot-pressed silicon nitride ceramics, 300
/
330 GPa [28], implying that the least-square regression
analysis method is suitable for the determination of the
Young’s modulus.
Note that the best-fit value of intercept in S -axis,
0.021 mN nm 1, is so large that it cannot be reasonably
neglected when compared with the smallest value of S
used in the regression analysis. This conflicts with Eq.
(9), which predicts that the S/hc line would pass
through the origin. Such a conflict can be explained
based on the consideration of the indenter tip rounding.
The best-fit results of the straight line shown in Fig. 8
can be described as
S 0:0014hc 0:0210:0014(hc 15): (11)
Eq. (11) means that, in order to make sure that the
straight line between S and hc passes through the origin,
a correct factor for the contact depth should be
incorporated. Such a correction factor has a small value,
15 nm, and can be considered as a rough measure of the
Fig. 8. Variation of the initial unloading stiffness, S , with the contact
depth at peak load, hc. Note that the best-fit line has an intercept very
close to the origin.
effect of indenter tip radius on the contact depth
measurement.
In continuation of the above analysis, it can be
inferred that the peak-load-dependence of the extracted
modulus shown in Fig. 7 may be attributed to the effect
of the indenter tip rounding.
5. Summary and conclusions
The nanohardness, H , and the Young’s modulus, E ,
of a hot-pressed silicon nitride were deduced by analyz-
ing the unloading segments of the nanoindentation
load
/displacement curves using the widely adopted
Oliver
/Pharr method. The variations of the resultant
H and E with the peak load employed to conduct the
nanoindentation tests were examined and the following
conclusions were obtained:
(1) The nanohardness, H, decreases with increasing
peak load, from 26 GPa at 8 mN to 19 GPa at 500 mN.
The peak-load-dependence of the nanohardness can be
well described with an empirical equation previously
established for the description of the ISE observed in
microhardness testing. The value of the load-indepen-
dent hardness deduced by analyzing the experimental
data according to the empirical equation is similar to
that of the microhardness measured in the load range
from 1 to 10 kg.
(2) The Young’s modulus, E , extracted directly using
the conventional stiffness equation, Eq. (9), also exhibits
a peak-load-dependence. As peak load increases from 8
to 500 mN, E decreases from 360 to 320 GPa. Such a
peak-load-dependence may be attributed to the effect of
indenter tip rounding. In order to obtain a reasonable,
peak-load-independent modulus, a new method was
proposed in which the modulus is determined directly
from the slope of the best-fit straight line between the
initial unloading stiffness, S , and the contact depth at
peak load, hc.
Acknowledgements
The support from the High-Tech Research and
Development Program of China (863 Program) under
grant 2001-AA-339010 is appreciated.
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