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ARB (Accumulative Roll-Bonding)
and other newTechniques to
Produce Bulk Ultrafine Grained
Materials
By Nobuhiro Tsuji,*Yoshihiro Saito, Seong-Hee Lee, and Yoritoshi Minamino
1. Introduction
Ultrafine grained (UFG) metallic materials whose mean
grain size is smaller than 1 lm are expected to perform prom-
inent mechanical properties. In order to put the UFG materi-
als to structural use, they must have bulky dimensions.
Severe plastic deformation (SPD) is a hopeful process to fabri-
cate bulky materials with submicrometer grain sizes. Before
SPD, grain refinement of metallic materials has been mainly
achieved by conventional plastic working and subsequent an-
nealing which results in recrystallization by nucleation and
growth (discontinuous recrystallization). The minimum grain
size achieved in this route has been about 10 lm. The total
reduction in conventional cold-rolling in industries, for exam-
ple, is 60 ~ 80 %, which corresponds with von Mises true
strain (e) of 1.06 ~ 1.86, while very large plastic strain over 4.0
is applied to the materials in the SPD processes, so that the
UFG microstructures form in the heavily deformed materials.
In recent years, various kinds of SPD processes have been
proposed and the research works on the SPD and the UFG
materials have been energetically conducted. In the present
paper, the authors try to overview the various SPD processes
for ultragrain refinement, especially putting stress on the
Accumulative Roll-Bonding (ARB) process
[13]
which is a
promising SPD process invented by the present authors for
bulky materials.
2. Various SPDProcesses
2.1. Two Successful SPD Processes
The most famous and successful SPD processes are the
equal channel angular extrusion (or pressing) (ECAE or
ECAP)
[4]
and the high pressure torsion (HPT)
[5]
whose out-
lines are illustrated in Figure 1. In ECAE, the material is put
into an angular channel-die and have a simple shear defor-
mation. The plastic strain per pass depends on the channel-
angle as well as the corner radius of the die, and typical
338 2003 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim DOI: 10.1002/adem.200310077 ADVANCED ENGINEERING MATERIALS 2003, 5, No. 5

[*] Prof. N. Tsuji*, Prof. Y. Saito*, Prof. Y. Minamino*

Osaka University
Suita 565-0871 (Japan)
E-mail: tsuji@ams.eng.osaka-u.ac.jp
Prof. S.-H. Lee
Mokpo National University
Mokpo 534-729 (Korea)
[**] The present work was financially supported by Industrial
Technology Research Grant Program '01 from NEDO of Japan
under project ID 01A23025d, Grant-in-Aid for Scientific
Research (No.14702052), and the 21st Century COE Program
Center of Excellence for Advanced Structural and Functional
Materials Design in Osaka University from the Ministry of
Education, Sports, Culture, Science and Technology of Japan.
Accumulative roll-Bonding (ARB) is a severe plastic deformation (SPD) process invented by the
authors in order to fabricate ultrafine grained metallic materials. ARB is the only SPD process applic-
able to continuous production of bulky materials. In the process, 50 % rolled material is cut into two,
stacked to be the initial dimension and then rolled again. In order to obtain one-body solid material,
the rolling in ARB is not only a deformation process but also a bonding process (roll-bonding). By
repeating this procedure, SPD of bulky materials can be realized. In this review paper, various kinds of
new SPD mechanical properties of the ARB processed materials are indicated.
Tsuji et al./Produce Bulk Ultrafine Grained Materials
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equivalent strain (e) in 90 die is about 1.0.
[6]
Because cross-
sectional area is constant after the pass, the procedures can be
repeated limitlessly so that large plastic strain is imposed on
the materials. Numerous numbers of researchers are now
studying the ECAE process all over the world, since it is easy
to install the process, which does not require special equip-
ments except for the dies and a press-machine, in the labora-
tories. The ECAE process has been applied to various kinds
of metals and alloys and succeeded in producing the UFG mi-
crostructures after several passes in most cases. However, the
major materials used are light metals like Al-alloys and Mg-
alloys and the trials for steels are limited.
[7,8]
This is presum-
ably because large force is required to put the materials
through the channel-die, overcoming large flow stress and
frictional stress. The hydrostatic compressive stress field in
the ECAE process is an advantageous point to prevent frac-
ture of the materials. However, cracking due to shear locali-
zation has been reported in less-workable materials such as
Ti-Al-V alloy.
[9]
Though the ECAE can certainly fabricate bulk
materials, typical size of the samples is still small. Further,
the ECAE is principally not a continuous process but a batch
process. Several trials for the continuous ECAE processing
have been done, as will be shown later. Disc sample is tor-
sionally deformed under high pressure of several GPa in the
HPT process.
[5]
Because of no change in the sample dimen-
sion, very large shear strain can be achieved along the periph-
ery. It should be noted, however, that the amount of shear
strain (so that the strain rate as well) differs depending on the
radial position. There is no hope for bulky applications of this
process, since the HPT can be applied only to small and thin
disc samples. However, the process might be scientifically
useful. For example, solid-state amorphization and nanocrys-
tallization of NiTi by this process has been recently report-
ed.
[10]
Because both of these successful SPD processes use
simple shear deformation principally, the role of shear for the
ultra-grain refinement has been argued. Although there are
still many unclear issues on the role of shear strain, the
authors think that the shear deformation is not necessarily re-
quired for the UFG formation. This is because the UFG micro-
structures can be produced by the ARB and the conventional
rolling, as will be discussed later. It is obvious, however, that
the primary important point in SPD is the deformation with-
out dimensional changes of the materials. Simple shear is a
deformation without change in height (thickness) of the mate-
rials, so that it is certainly advantageous for SPD.
2.2. Continuous ECAE Processes
From a viewpoint of practical application, one of the most
disadvantageous points in the ECAE process is that it is not a
continuous process but a batch process, as was pointed out
above. A few experiments to make the ECAE continuous
have been attempted (Fig. 2). Saito et al.
[11,12]
developed the
Conshearing process for continuous ECAE of sheet metals
(Fig. 2a). They equipped the ECAE die at the end of the Satel-
liteMill they previously invented.
[13]
The SatelliteMill is the
special rolling mill which can make the rotating speed of all
the satellite rolls constant. As a result, compression force
along the rolling direction (RD) appears in the materials be-
tween adjacent satellite rolls. Folding of the materials is pre-
vented by the guideshoe equipped between the satellite rolls.
They used the compression force in the SatelliteMill to put
the sheet into the ECAE die. The Conshearing was applied to
a commercial purity aluminum up to 4 cycles and succeeded
in fabricating sound sheets, but UFG microstructures have
not been obtained.
[12]
Because they used sheet materials, it
was probably not effective to impose ideal shear strain owing
to the bending and bending-back deformation, and friction.
[12]
Further, it is difficult to make the channel-angle 90 in this
configuration (they used 125)
[11,12]
On the other hand, the
processed materials showed unique textures.
[11]
Lee et al.
[14]
developed another continuous ECAE process, named the con-
tinuous confined strip shearing (C2S2) process, which is prin-
cipally the same as the conshearing. They seem to use con-
ventional two-high mill, but the surface of the lower roll was
mechanically roughened in order to feed the material into the
ECAE die. As a result, the surface quality of the specimens
would be worse than the conventionally rolled materials. The
strips with a dimension of 1.55
T
20
W
1000
L
mm
3
were pro-
cessed by the C2S2 process and the UFGs similar to those
obtained in the conventional ECAE have been reported in
1050-Al, though the difficulties and the disadvantages are not
obvious from the limited publications at the present moment.
The channel-angle was varied from 100 to 140, and it was
found that the critical strain to form the UFGs increases with
increasing the angle.
[14]
2.3. Other Processes
Other unique SPD processes are summarized in Figure 3.
Their main concept is the repetition of plastic deformation
without change in the dimension of the materials, which is
ADVANCED ENGINEERING MATERIALS 2003, 5, No. 5 http://www.aem-journal.de 2003 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 339
(a) (b)
Fig. 1. Outlines of a) ECAE and b) HPT processes.
(a) (b)
Fig. 2. Outlines of a) Conshearing and b) C2S2 processes.
Tsuji et al./Produce Bulk Ultrafine Grained Materials
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common in all the special SPD processes. The cyclic extrusion
compression (CEC; Fig. 3a) is a repetition of the extrusion to
decrease the sample diameter and the compression to in-
crease the diameter to the initial dimension.
[15,16]
The hydro-
static compressive stress field in the process would be prefer-
able to avoid fracture of the materials, although it must be a
batch process for the materials with limited sizes. There are
only limited number of reports about ultra-grain refinement
by the CEC process,
[17]
but bulk mechanical alloying of Ag-
70at.%Cu has been achieved.
[16]
Figure 3b shows the outline
of the continuous cyclic bending (CCB) process proposed by
Takayama et al..
[18]
This is a repetition of bending and bend-
ing-back. Though the maximum strain at the surface achieved
in the single bending pass is small (e =0.1056),
[18]
it is very
easy to repeat the process and then large total strain can be
summed after many passes. However, UFG microstructures
have not been developed by this process. The results of this
attempt can suggest us two significant points: i) Even if large
amount of total strain is imposed as a summation of small
strain, UFGs do not necessarily form in the materials. ii) Re-
turning deformation, like bending and bending back in the
CCB, seems disadvantageous for ultra-grain refinement. Re-
cently, a new SPD process which seems hopeful for continu-
ous production of bulky UFG materials has been pro-
posed.
[19,20]
It is the repetitive corrugation and straightening
(RCS) process illustrated in Figure 3c. The process illustrated
in Figure 3c is, however, still in imagination, and the actual
experiments are simulated in simple bending by use of a
pressing machine equipped with dies.
[19,20]
Although the
principle of the RCS is bending and bending-back, which is
the same as the CCB, the UFG microstructure was reported in
RCS processed Cu.
[20]
Probably the difference between the
CCB and the RCS is the amount of strain per pass. However,
when the strain per pass is increased by reducing the corner
radius of the tools, the strain must inevitably localize in lim-
ited parts of the materials depending on the radius of the
tools (dies). It is also the case even if the continuous process
illustrated in Figure 3c could be realized.
3. Accumulative Roll-Bonding (ARB)
3.1. Principle of the ARB
The accumulative roll-bonding (ARB)
[13]
is an only SPD
process using rolling deformation itself. The ARB was in-
vented by the present authors in 1998.
[1]
The principle of the
ARB is illustrated in Figure 4. Rolling is the most advanta-
geous metalworking process for continuous production of
plates, sheets and bars. However, the total reduction applied
to the materials is substantially limited because of the de-
crease in the cross-sectional dimension of the materials with
increasing the reduction. In the ARB process, 50 % rolled
sheet, for example, is cut into two, stacked to be the initial di-
mension, and then rolled again. In order to obtain one-body
solid materials, the rolling in the ARB is not only a deforma-
tion process but also a bonding process (roll-bonding). To
achieve good bonding, the surface of the materials is de-
greased and wirebrushed before stacking, and the roll-bond-
ing is sometimes carried out at elevated temperatures below
340 2003 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim http://www.aem-journal.de ADVANCED ENGINEERING MATERIALS 2003, 5, No. 5
(a) (c) (b)
Fig. 3. Outlines of a) CEC, b) CCB, and c) RCS processes.
Fig. 4. Schematic illustration showing the principle of the accumulative roll-bonding
(ARB) process.
Table 1. Geometrical changes of the materials during the ARB where two pieces of the sheets 1mm thick are roll-bonded by
50 % reduction per cycle.
No. of cycles 1 2 3 4 5 6 7 8 9 10 n
No. of layers 2 4 8 16 32 64 128 256 512 1024 2
n
No of bonded
boundaries
1 3 7 15 31 63 127 255 511 1023 2
n
1
Layer interval (lm) 500 250 125 62.5 31.2 15.6 7.8 3.9 1.9 0.96 1000/2
n
Total reduction (%) 50 75 87.5 93.8 96.9 98.4 99.2 99.6 99.8 99.9 (1 1/2
n
) 100
Equivalent strain 0.8 1.6 2.4 3.2 4.0 4.8 5.6 6.4 7.2 8.0

3
p ln 2

n = 0.8 n
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the recrystallization temperature of the materials. Since the
above mentioned procedures can be repeated limitlessly, it is
possible to impose very large plastic strain on the materials in
the ARB process. Table 1 summarizes the geometrical
changes of the samples during the ARB, provided two pieces
of the sheets 1 mm thick are stacked and roll-bonded by 50 %
reduction per cycle. It is interesting that the number of the ini-
tial sheets included in the sheet ARB processed by n cycles
becomes 2
n
. For example, 1024 initial sheets are included in
the 10-cycles ARB processed materials, so that the mean
thickness of the initial sheet is smaller than 1 lm. Because
von Mises equivalent strain of the 50 % rolling is 0.80, the to-
tal equivalent strain after n cycles is 0.8 n. It has been found
by our studies that bonding in the ARB process is not difficult
generally. For example, good bonding of low-carbon steel can
be achieved even at ambient temperatures.
[3]
However, sur-
face treatment is indispensable for bonding. Furthermore,
there is a critical rolling reduction in one pass roll-bonding,
below which it is difficult to achieve sufficient bonding.
Though the critical reduction depends on the materials and
the processing temperatures, more than 35 % reduction by
one pass is necessary in general, so that the rolling-force be-
comes big compared with the conventional rolling. Except for
the enough capacity of the rolling mill which can realize one-
pass heavy roll-bonding, there are no special requirements in
the equipments for the ARB. The serious problem in the ARB
process is fracture of the materials.
[3]
Because large amount of
total plastic strain is accumulated in the materials and the
rolling is not a hydrostatic process, edge-cracks sometimes
occur in the sheets especially at higher cycles. In certain kinds
of the materials, such as AlMg alloy, the edge cracks greatly
propagate into the centre of the sheets. In that case, it be-
comes impossible to proceed to the subsequent cycles. How-
ever, there are several small techniques to avoid such crack-
ing, and the sound bulky sheets can be fabricated by the ARB
process in most of the metallic materials.
[13,2134]
In cases of
quite ductile materials, for example, pure aluminum and iron,
the UFG sheets having a dimension of 1
T
50
W
300
L
mm
3
can be fabricated without cracking by the ARB process even
in the university laboratories.
[3]
3.2. ARB Processed Materials
The materials ARB processed by several cycles are filled
with the UFGs. Figure 5 shows the TEM microstructures indi-
cating the typical UFGs in various kinds of the ARB pro-
cessed Alalloys and steels.
[3]
Independent of the kind of the
materials, the clear UFGs whose diameters are smaller than
1 lm are observed. The UFGs are surrounded by clear but ir-
regular shaped boundaries and the number of dislocations in-
side the grains seems small. These features are similar to
those observed in the materials heavily deformed by other
SPD processes. It should be noted, however, the microstruc-
ADVANCED ENGINEERING MATERIALS 2003, 5, No. 5 http://www.aem-journal.de 2003 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 341
Fig. 5. TEM microstructures of the typical UFGs in various kinds of ARB processed
materials. Observed from ND. a) 1100-Al (99 %Al) ARB processed by 8 cycles
(e =6.4) at 473 K. b) 5083-Al (Al-4.5 %Mg) ARB processed by 7 cycles (e =5.6) at
573 K. c) 6061-Al (Al-1.1 %Mg0.4 %Si) ARB processed by 6 cycles (e =4.8) at RT.
d) 7N01-Al (Al-4.4 %Zn-1.8 %Mg) ARB processed by 5 cycles (e =4.0) at 523 K and
then annealed at 473 K for 900 s. e) IF steel ARB processed by 5 cycles (e =4.0) at
773 K, and then annealed at 773 K for 600 s. f) Plain low-carbon steel (SS400; Fe-
0.13 %C-0.37 %Mn) ARB processed to a total strain of 4.0 at RT., and annealed at
833 K for 1.8 ks.
(a)
(b)
Fig. 6. TEM image a) and corresponding misorientation map b) of the IF steel ARB
processed by 7 cycles (e =5.6) at 773 K. Observed from TD. The misorientations (deg.)
indicated in b) were calculated from the accurate orientations of the elongated grains
measured by TEM/Kikuchi-line analysis.
Tsuji et al./Produce Bulk Ultrafine Grained Materials
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tures in Figure 5 were observed from the normal direction
(ND) of the sheets. The most characteristic feature of the
UFGs in the ARB processed materials is the elongated mor-
phology. Figure 6a is a typical microstructure of the elon-
gated ultrafine grains in the ultra-low-carbon IF (interstitial
free) steel ARB processed by seven cycles (e =5.6) at
500 C.
[3,26,30]
The grains are elongated along RD. Quite similar
microstructures appear in the ARB processed aluminum al-
loys.
[3,25,29]
These microstructures resemble the lamellar bound-
ary structures observed in heavily deformed materials.
[35]
Fig-
ure 6b is the misorientation map of the identical regions
obtained by TEM/Kikuchi-line analysis.
[36]
Such orientation
measurements clearly confirm that the elongated UFGs are
not subgrains but grains surrounded by highangle grain
boundaries. The high density of the high-angle grain bound-
aries in the ARB processed materials has been also confirmed
in macroscopic regions by means of SEM/EBSD analysis.
[30]
At the same time, however, the UFGs have characteristics as
deformation microstructures, such as the elongated grain
shape and the dislocation substructures inside the grains. The
formation mechanism of the UFGs during SPD is still an issue
under discussion. However, recent investigations suggest
that the formation process of the UFGs is not conventional
discontinuous recrystallization but continuous recrystallization
(or in-situ recrystallization) characterized by ultrafine grain
subdivision, recovery to form clear UFGs, and short range
grain boundary migration.
[37,38]
The ARB processed materials
having the elongated UFG structures perform very high
strength.
[1,3,21,24,25,27,31,32]
The grain size and the tensile strength
of the various UFG materials fabricated by the ARB are sum-
marized in Table 2. In most cases, the mean grain thickness of
the pancake-shaped UFGs or the ultrafine lamellar structures
are 100 ~ 200 nm. The materials with higher purity tend to
show larger grain size. The ARB at lower temperature results
in smaller grain size within the similar materials. The UFG
materials perform the tensile strength two to four times high-
er than those of the starting materials having conventional
grain sizes. On the other hand, the ARB processed materials
have limited tensile elongation owing to early plastic instabil-
ity.
[31]
It has been also clarified that the ARB processed 5083-
Al alloy with UFG microstructure performs low-temperature
superplasticity at 200 C.
[22,23]
3.3. Role of Redundant Shear in the ARB
The UFG microstructures are likely to be
formed by the ultrafine grain subdivision
during SPD principally.
[37]
As a result, the
elongated UFG structures in the ARB pro-
cessed materials are quite similar to the la-
mellar boundary structures which have been
observed in the materials heavily deformed
by conventional rolling.
[35]
This indicates
that the UFG structures are formed not only
342 2003 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim http://www.aem-journal.de ADVANCED ENGINEERING MATERIALS 2003, 5, No. 5
Table 2. Microstructure, grain size and tensile strength of the various kinds of metals and alloys ARB processed in Osaka Univer-
sity.
Materials
[mass %]
ARB Process Microstructure Grain size
[lm]
Tensile strength
[MPa]
4N-Al 7 cycles at RT pancake UFG 0.67 125
100-Al (99 % Al) 8 cycles at RT pancake UFG 0.21 310
5052-Al (Al-2.4Mg) 4 cycles at RT ultrafine lamellae 0.26 388
5083-Al (al-4.5Mg+0.57Mn) 7 cycles at 100C ultrafine lamellae 0.08 530
6061-Al (Al-1.1Mg-0.63Si) 8 cycles at RT ultrafine lamellae 0.10 357
7075-Al (Al-5.6Zn-2.6Mg-1.7Cu) 5 cycles at 250C pancake UFG 0.30 376
OFHC-Cu 6 cycles at RT ultrafine lamellae 0.26 520
Cu-0.27Co-0.09P 8 cycles at 200C ultrafine lamellae 0.15 470
Ni 5 cycles at RT ultrafine lamellae 0.14 885
IF steel 7 cycles at 500C pancake UFG 0.21 870
0.041P-IF 5 cycles at 400C pancake UFG 0.18 820
SS400 steel (Fe-0.13C-0.37Mn) 5 cycles at RT ultrafine lamellae 0.11 1030
Fe-36Ni 7 cycles at 500C ultrafine lamellae 0.087 780
Fig. 7. Optical microstructures showing the flection of the embedded pin in the 1100 aluminum sheet ARB pro-
cessed by one cycle at ambient temperature without lubrication. Observed on a longitudinal cross-section.
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by shear deformation like ECAE and HPT but also by another
mode of plastic deformation, such as rolling (ARB). However,
Huang et al.
[29]
recently clarified that the formation of the ul-
trafine structure is much faster in the ARB processed 99 % Al
than that in the conventionally rolled 99 % Al. For example,
the mean misorientations in the ARB processed specimen is
significantly larger than that in the conventionally cold-rolled
specimen at the identical strains.
[29]
This means that the ARB
process is more advantageous for ultra-grain refinement than
the conventional rolling. A probable reason for this difference
between the ARB and the conventional rolling is the redun-
dant shear strain. The roll-bonding in the ARB process has
been usually carried out without lubrication. It has been
known that large amount of redundant shear strain is applied
at subsurface regions of the sheets in the rolling under the
less-lubricated conditions.
[39]
In the ARB of 1100-Al, the re-
dundant shear strain has been quantitatively evaluated by
Lee et al.
[28]
Figure 7 shows the flection of the embedded pin
after the 1st cycle of the ARB. The straight pin embedded ver-
tically to the sheet before roll-bonding has been greatly bent
especially near the surface, which indicates large redundant
shear strain was imposed due to large friction between the
rolls and the specimen. The shear strain (e) distribution
through thickness, which was calculated from the flection in
Figure 7, is shown in Figure 8a.
[28]
The shear strain (c) just be-
low the surface reaches up to 8 (e =4.6). It has been also clari-
fied that the subsurface regions of the ARB processed sheets
have a kind of shear texture completely different from the
center regions.
[1,30]
The characteristic in the ARB processed
sheet is the complicated distributions of the redundant shear
strain after several cycles, as is shown in Figure 8. Because
the 50 % rolled sheet is cut and stacked between cycles, half
of the surface which had undergone the severe shear defor-
mation comes into the center. As a result, different from con-
ventional rolling, the sheared regions do not localize only at
subsurface layers but complicatedly distribute through thick-
ness of the sheets as the ARB cycle proceeds (Fig. 8). Because
shear deformation does not change the thickness of the mate-
rials, the integrated area in Figure 8 (integrated shear strain)
should be added to the equivalent strain of the sheet. That is,
the substantial strain applied during the n-cycles of the ARB
without lubrication is much larger than 0.8 n, which was cal-
culated only from the reduction in thickness. The substan-
tially larger strains accumulated must be one of the reasons
for the faster development of the UFG structure in the ARB
materials. Furthermore, the effect of changing strain path
should be taken into account as well. The ARB processed ma-
terials have had quite complicated combination of plane-
strain deformation and shear deformation, depending on the
thickness location and the number of cycles. This means that
the strain path at each region greatly changes between shear
and plane-strain compression in every cycle. As a result, the
centre part of the ARB processed sheets show relatively weak
texture even after large rolling reduction. Although the role
of the strain path for ultra-grain refinement is still under dis-
cussion, the present results in the ARB suggests that changing
the strain path is effective for the formation of the UFGs, in
other words, for the faster ultrafine grain subdivision.
4. Summary
Various kinds of SPD processes were overviewed and the
characteristics of the ARB process was summarized. The for-
mation of the UFG structure was discussed, putting stress on
the role of shear deformation. It was shown that the ARB is
the promising SPD process which can produce the bulky
UFG materials continuously. By use of the advantages in the
ARB process, formation mechanism of the UFGs as well as
the properties of the UFG materials should be further studied
in the future.
Received: March 4, 2003

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