Scripta Materialia 46 (2002) 383–388

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Formation of nanocrystalline structure in steels by ball

drop test
M. Umemoto a,*, B. Huang a,b, K. Tsuchiya a, N. Suzuki a
a
Department of Production Systems Engineering, Toyohashi University of Technology, Tempaku-cho, 1-1 Hibarigo-oka,
Toyohashi, Aichi 441-8580, Japan
b
Institute of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200030, China
Received 26 October 2001; received in revised form 9 November 2001; accepted 3 December 2001

Abstract
Formation of nanocrystalline structure in a eutectoid steel by severe plastic deformation has been studied by a ‘ball
drop test’. The microstructures and hardness similar to those of nanocrystalline structures produced by ball milling
have been obtained near the surface of specimens. The high strain rate of around 104 s
1 is proposed to be an essential
condition to produce nanostructure by deformation. Ó 2002 Acta Materialia Inc. Published by Elsevier Science Ltd. All
rights reserved.

Keywords: Cold working; Microstructure; Steel; Nanocrystalline

1. Introduction torsion straining (SPTS) [4] and accumulative roll

Nanocrystalline materials have been attracting
increasing interests, since the grain size in the na-
nometer range leads to various unusual proper-
ties. Various methods have been used to produce
nanocrystalline materials, such as inert gas con-
solidation, mechanical alloying, physical vapor
deposition, sol–gel process, chemical vapor depo-
sition, etc. To produce large volume of nanocrys-
talline materials, the processes involving heavy
deformation, such as ball milling (BM) [1,2], equal
channel angular pressing (ECAP) [3], severe plastic
*
Corresponding author. Tel.: +81-532-44-6709; fax: +81-
532-44-6690.
E-mail address: umemoto@martens.tutpse.tut.ac.jp (M.
Umemoto).
bonding (ARB) [5,6] have been proposed. Among
these, extensive works have been performed on the
formation of nanocrystalline structures by BM due
to its simplicity, low cost, and applicability to es-
sentially all classes of materials. In our previous
papers [7–11], we have reported the microstruc-
tural evolution and nanocrystallization of Fe–C
alloys by BM. It was found that the nanocrystal-
lization in the Fe–C alloys starts from the surface
of powders and develops into the interior. Both
the structures and hardness in the nanocrystalline
region are clearly different from those in the
work-hardened region. The boundary between the
nanocrystalline and work-hardened regions is
quite sharp. To induce nanocrystallization by de-
formation a critical dislocation density is consid-
ered to be required [7–11]. High strain rate may be
one of the necessary conditions to achieve this

1359-6462/02/$ - see front matter Ó 2002 Acta Materialia Inc. Published by Elsevier Science Ltd. All rights reserved.
PII: S 1 3 5 9 - 6 4 6 2 ( 0 1 ) 0 1 2 5 8 - 1
384 M. Umemoto et al. / Scripta Materialia 46 (2002) 383–388

critical dislocation density [4,10,11]. However, in a

BM process, deformation mode is substantially
complicated and contamination from the vial or
atmosphere is difficult to avoid. To overcome these
difficulties an experiment using a falling-ball im-
pact wear tester to simulate the conditions of BM
has been conducted by Zhang et al. [12]. A cast
iron ball was dropped on a steel sample. They
observed white layers with fine subgrains both on
the surface and interior of the sample. They con-
sidered that the observed white layers are adiabatic
shear bands and the subgrains are formed by dy-
namic recovery. However, the comparison with
BM is missing.
In the present study, a ball drop test, in which a
ball with a weight was dropped onto the surface of
a flat bulk specimen, was carried out. High strain
Fig. 1. Schematic drawing of the ball drop test.
rate around 104 s
1 similar to that in BM was
considered to be achieved with this simple test.
Nanocrystalline structures similar to the one ob- scanning electron microscope (JEOL JSM-6300),
tained by BM was observed in the specimens after transmission electron microscope (Hitachi H-800
a number of ball drops. This provides better un- working at 200 kV) and microvickers hardness
derstanding of the nanocrystallization mechanism tester (MVK-G1 with an applied load of 9.8 N for
by severe plastic deformation. 10 s). Specimens for SEM observations were
etched by 5% Nital. Thin foils for TEM observa-
tions were prepared by cutting a specimen parallel
2. Experimental procedures to its surface into discs of 3 mm in diameter using
a wire spark cutting machine (brother HS-300) and
The material used in the present study was a then dimpling from the bottom side which is fol-
carbon steel with a slightly hypereutectoid com- lowed by ion beam thinning.
position (Fe–0.89C–0.25Si–0.50Mn in mass%) with
pearlite or spheroidite structures. The pearlite
structure was obtained by austenitizing the sample 3. Results and discussion
at 1223 K for 1.8 ks and then kept at 873 K for 0.3
ks. To obtain spheroidite structure, specimens 3.1. Ball drop test for specimens with pearlite
were austenitized at 1173 K for 3.6 ks and quen- structure
ched into water to obtain martensite. Such speci-
mens were tempered at 983 K for 79.2 ks. Fig. 2(a) is a SEM micrograph of a cross-sec-
Schematic drawing of the ball drop test is tion of the specimen with pearlite structure after 50
shown in Fig. 1. A weight with a ball attached on times of ball drops with a weight of 3 kg. A layer
its bottom was dropped from a height of 1 m onto with dark appearance (appears white under an
a bulk specimen with flat surface. The ball of 6 mm optical microscope) with a thickness of about 10
in diameter and the weights of either 3, 4 or 5 kg lm is seen along the surface of the specimen. The
was used. The specimen with 15 mm in diameter lamellar structure of pearlite cannot be seen in the
and 4 or 8 mm in thickness was set in a ring which dark layer. Under this layer, deformed lamellar
prevents deformation in the radial direction. All structure of pearlite is clearly observed (this region
the tests were carried out at room temperature in is hereafter referred to as work-hardened region).
air. Deformed specimens were characterized by a The microhardness of the dark layer is as high as
 M. Umemoto et al. / Scripta Materialia 46 (2002) 383–388
Fig. 2. SEM images of Fe–0.89C pearlite steel after ball drop of (a) 50 times with a weight of 3 kg, (b) 10 times with a weight of 5 kg.
9.4 GPa, which is much higher than that of the
work-hardened region (4.5 GPa). It was noted that
the observed microstructures after the ball drop
test were similar to those observed in ball milled
powders with pearlite structure. In the ball milled
powder, dark layer was also observed near the
surface of the powders and the work-hardened
region was observed in the interior of the powder.
It was also revealed that the dark layer consists of
either equiaxed or elongated grains with an aver-
age size around 20 nm and the microhardness is
around 9.4 GPa [8,11], which agrees with that
observed in the present ball drop test. Therefore,
the dark layer observed in the specimen after the
ball drop test is considered to be nanocrystalline
ferrite.
The dark layer (nanocrystalline ferrite region)
was found not only along the surface of the spec-
imen but also in the region several tens of mi-
crometers below the specimen surface as shown in
Fig. 2(b). In most cases, the dark nanocrystalline
layer was seen parallel to the specimen surface. It
was considered that nanocrystalline structure is
produced in the region where the most severe de-
formation occurred. In the case of the ball drop
test, the degree of deformation may not be always
the largest at the surface of the specimen because
of the friction between the specimen and ball. This
might be the reason why dark layers form in the
interior of the specimen.
Fig. 3 shows a dark field image and electron
diffraction pattern of a sample with pearlite
structure after ball dropped 25 times with a weight
385
of 4 kg. The dark field image of Fig. 3 (taken using
the (1 1 0) ring of the ferrite) shows that the ferrite
grain size is of the order of 100 nm. All the dif-
fraction rings correspond to those of the bcc ferrite
and rings corresponding to cementite are hardly
detected. This indicates that the cementite is
mostly dissolved into the ferrite matrix. The dif-
fraction pattern was obtained from the area of
2 lm Ø and shows nearly continuous rings, indi-
cating the random orientations of ferrite grains.
3.2. Ball drop test for specimens with spheroidite
structure
Similar microstructural changes with those in
the specimen with the pearlite structure were ob-
served in the specimens with spheroidite structure
by the ball drop test. Fig. 4(a) shows a micro-
structure of a specimen ball dropped 50 times with
a weight of 2 kg. The uniform structured layer is
seen along the specimen surface. The microhard-
ness of this region is 8.8 GPa which is much higher
than the interior work-hardened region (5.5 GPa).
The highest microhardness of the uniform struc-
tured layer in the ball dropped specimen (after
eight times drops) was 9.6 GPa, which agrees with
that observed in the ball milled powder (9.5 GPa),
in which the average grain size of about 20 nm was
observed by TEM [11]. It should be noted that
cementite particles are hardly observed in the
uniform structured layer but remain undeformed
in the work-hardened region. The uniform struc-
tured layer was also observed in the interior of the
386 M. Umemoto et al. / Scripta Materialia 46 (2002) 383–388

Fig. 3. A dark field image and electron diffraction pattern of Fe–0.89C pearlite steel after ball drop of 25 times with a weight of 4 kg.

Fig. 4. SEM images of Fe–0.89C spheroidite steel after ball drop of (a) 50 times with a weight of 2 kg, (b) 3 times with a weight of 4 kg.

ball dropped specimen as shown in Fig. 4(b). In
the uniform structured layer, many wavy bands
parallel to each other are seen together with sphe-
roidal cementite. The density of wavy bands near
the center is higher and it looks like they coalesce
with each other. The observed microstructures are
quite similar to those of corresponding ball milled
samples [11]. At the initial stage of BM, a submi-
cron wavy band structure forms near the surface of
a powder particle. With increasing milling time,
volume fraction of the wavy band structure in-
creases and they evolve into a uniform nanocrys-
talline ferrite. Longer milling time up to 1800 ks
leads to complete dissolution of cementite and the
formation of a uniform nanocrystalline structure in
the whole particles.
4. Ball press test
It was considered that high strain rate is one of
the necessary conditions to obtain nanocrystalline
structure by heavy deformation. To confirm this, a
ball press test was carried out. The specimens used
for ball press test were compressed using the same
steel ball (Fe–1.0C–1.5Cr, SUJ2) with a diameter
of 6 mm. Similar degree of deformation was ap-
plied by a number of compressions on the speci-
 M. Umemoto et al. / Scripta Materialia 46 (2002) 383–388
men surface with a load of 2000 kgf. Each com-
pression was carried out for about 1 s (this cor-
responds to the strain rate of about 1 s
1 ). The
structure observation and microhardness mea-
surement revealed that there was no trace of
nanocrystalline structure even after the specimen
was compressed 50 times.
5. Discussion
Zhang et al. [12] have carried out an experiment
using the falling-ball impact wear tester to simu-
late the deformation conditions of BM. A cast iron
ball of 4 kg (100 mm in diameter) was dropped 30
times from a height of 3.5 m on a tempered low
alloy 0.4 mass% C steel sample with the angle of
45°. They reported that a white layer with fine
subgrains was observed on the surface and interior
of sample. The structures they observed are similar
to those obtained in the present study. However,
they did not examine the deformation conditions
in their experiment, such as the degree of defor-
mation or strain rate. The present deformation
condition is analyzed as follows.
When a ball of 6 mm in diameter with a weight
of 4 kg was dropped from the height of 1 m onto a
flat bulk specimen surface, the potential energy E
of the weight (¼ mgH , where m is the mass of
weight and H is the height) is 39.2 J. The velocity
pffiffiffiffiffiffiffiffiffi
of the ball when it hits the specimen v0 (¼ 2gH )
is 4.4 m s
1 . The collision time s (¼ S=v, where S
is the collision depth (measured as 1.1 mm) and
v is the average velocity (0.5v0 ) of the ball dur-
ing collision) is 5  10
4 s. The collision load P
(¼ ma ¼ mv0 =s) is obtained as 3:6  103 kgf. The
average collision stress r (¼ P =A, where the con-
tact area A was measured as 21 mm2 ) is 1.7 GPa. It
should be noted that the collision time of 5  10
4
s is much shorter than that of the ball press test
(1 s) and the collision load of 3:6  103 kgf is 1.8
times larger than the load (2000 kgf) applied in the
ball press test. The strain rate by ball drop test can
be estimated as follows. For the 0.89C pearlite
steel, the measured relationship between the stress
(r) and plastic strain (e) is rðMPaÞ ¼ 1000 þ 250e.
Therefore, the energy per volume necessary to give
true strain e is obtained by integrating r and de
387
over the e as 1000e þ 125e2 (106 J m
3 ). If all the
potential energy of the weight is used for the
plastic deformation of a sample, 39:2 ¼ ð1000e þ
125e2 Þ  106  V , where V is the plastically de-
formed volume. If the plastically deformed volume
is assumed to be same with the volume of the
crater produced by a single ball drop test
(V ¼ 10
8 m3 ), the average plastic strain of 2.5 is
obtained. Consequently, an average strain rate
e_ ¼ e=s ¼ 5  103 s
1 . The strain rate in the ball
drop test is about 2000 times higher than that in
the ball press test.
Dissipation of the potential energy leads to a
temperature rise in plastically deformed region.
For the presentpexperiment,
ffiffiffiffiffiffiffi the thermal diffusion
distance R (¼ Dt s, where the thermal diffusion
coefficient Dt ¼ 4  10
6 m2 s
1 for steel and the
collision time s ¼ 5  10
4 s) is estimated to be 50
lm. This is much smaller than the plastically de-
formed thickness (1 mm). Thus thermal diffusion
can be neglected for the maximum temperature
reached. If all the potential energy of the weight is
converted into heat, average temperature rise is:
mgH
DT ¼ ;
vqm
where v is the heat capacity, q is the density. The
average temperature rise of 1140 K (v ¼ 444
J kg
1 K
1 and q ¼ 7:85 g cm
3 ) can be obtained.
This is considered to be the maximum temperature
rise that can be reached. A part of the potential
energy of the weight will be used for the bouncing
back of the weight, kinetic energy of the specimen
and specimen holder, sound, elastic energy of the
weight, and specimen, etc. Thus the actual tem-
perature rise may be about half of the above esti-
mated maximum temperature rise. However, the
possibility of local temperature raise above the
austenite transformation temperature (1000 K)
still remains. This means that there is a possibility
that the layered nanocrystalline ferrite is the mar-
tensite produced during cooling from the austenite
state. At present, there is no clear evidence to
support the occurrence of the transformation to
austenite by deformation induced heating.
Lee and Lam [13] have studied the deformation
behavior of high strength steels under various high
strain rates (103 to 5  103 s
1 ). They have found
388 M. Umemoto et al. / Scripta Materialia 46 (2002) 383–388
that the strain rate has an effect both on disloca-
tion arrangement and cell size. They also found
that the dislocation density at a given degree of
deformation increases with increasing strain rate.
With increasing the strain rate, dislocation cell size
decreases and fraction of cells with large misori-
entation increases [13]. From this experiment, it
can be inferred that when the strain rate is higher
than a certain value, the dislocation density can
reach a critical value to induce the transition from
dislocation cellular structure to granular struc-
ture (dynamic continuous recrystallization [14]). It
seems that high strain rate raises local temperature
and thermally assisted process may occur in some
extent. This might be the reason for that a high
strain rate is a necessary condition to produce
nanocrystalline structure as confirmed in the pre-
sent study.
6. Conclusions
To clarify the nanocrystallization mechanism
by BM, a ball drop test in which a ball with weight
was dropped onto a bulk specimen was carried
out. By this test heavy deformation with a high
strain rate similar to those in BM process (the es-
timated true strain of around 2 and strain rate of
104 s
1 ) may have been achieved. After the ball
drop test on eutectoid steel specimens, similar
microstructures and hardness with those in nano-
crystalline structures observed in the ball milled
powders were obtained. The formation of nano-
crystalline ferrite with the grain size of the order of
100 nm was confirmed by TEM observations. It
was noticed that nanocrystallization starts even
after a few times of ball drops. The present ex-
periment supports that in the nanocrystallization
by BM, the contamination has only a minor effect.
A large number of repeated deformation may not
be necessary and a few times of large deformation
can induce nanocrystallization if the strain rate is
high around 104 s
1 .
Acknowledgements
One of the authors (B. Huang) would like to
thank Heiwa Nakajima foundation for supplying
the scholarship to carry out this work in Japan.
This study is financially supported in part by the
Grant-in-Aid by the Japan Society for the Pro-
motion of Science.
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