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Materials and Design 32 (2011) 3280–3286

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Materials and Design


journal homepage: www.elsevier.com/locate/matdes

The effect of constrained groove pressing on grain size, dislocation density


and electrical resistivity of low carbon steel
F. Khodabakhshi, M. Kazeminezhad ⇑
Department of Materials Science and Engineering, Sharif University of Technology, Azadi Ave., Tehran, Iran

a r t i c l e i n f o a b s t r a c t

Article history: In this research, constrained groove pressing (CGP) technique is used for imposing severe plastic defor-
Received 29 October 2010 mation (SPD) on the low carbon steel sheets. Using transmission electron microscopy (TEM), X-ray dif-
Accepted 11 February 2011 fraction (XRD) and optical microscopy, the microstructural characteristics of produced sheets are
Available online 18 February 2011
investigated. The results show that CGP process can effectively refine the coarse-grained structure to
an ultrafine grain range. Dislocation densities of the ultrafine grained low carbon steel sheets are quan-
Keywords: titatively calculated and it is found that the CGP can effectively enhance the dislocation density of the
A. Ferrous metals and alloys
sheets. Measurements of their electrical resistivity values show that microstructure refinement and
C. Forming
E. Electrical
increasing the dislocation density can efficiently increase the electrical resistivity of the CGPed sheets
up to 100%.
Ó 2011 Elsevier Ltd. All rights reserved.

1. Introduction due to severe plastic deformation [9] and therefore, it seems that
more works should be carried out to investigate the relationship
Microstructure of materials can greatly affect their mechanical between microstructure evolution due to SPD and changes in phys-
and physical properties such as hardness, strength, electrical resis- ical properties. Electrical resistivity is one of the most important
tivity, thermal conductivity, and magnetic properties. Many works physical properties because its measurement is easy and also, it
have been carried out [1–4] on the relationship between micro- represents the variations of many other physical properties such
structure and physical properties for different materials. Recently, as electrical and thermal conductivity. Also, the electrical resistiv-
nano-structured (NS) materials have been mostly attracted in ity has been used in many researches as a tool for determining the
materials science due to their unique properties and behavior. microstructural phenomenon occurs in different processes. Previ-
These materials are defined as solids having microstructure fea- ous researches show that the grain size is decreased and the dislo-
tures in the range of nanometer, at least in one dimension [5]. cation density is significantly increased through SPD of metals
Two complementary approaches have been developed to synthe- [6,7]. Also, it has been shown that a smaller grain size leads to low-
size NS solids. The first is the ‘‘bottom–up’’ approach in which bulk er thermal conductivity and higher electrical resistivity due to en-
NS materials are assembled from individual atoms or nano-scaled hanced phonon boundary scattering at interfaces and crystal
blocks such as nano-particles. The second approach is the ‘‘top- imperfections such as dislocations [10]. It has been shown that
down’’ approach in which existing coarse-grained materials are the electrical resistivity of a copper superconductor is mainly
processed to produce nano-structured materials. The most suc- dependent on the surface of grain boundaries and concentration
cessful ‘‘top–down’’ approach involves the use of severe plastic of second phase precipitations [11]. Since microstructure is refined
deformation in which materials are subjected to the very large during SPD and microstructural evolution can affect the electrical
strains without changes in the cross-sectional dimensions of the resistivity changes, therefore, it seems that an investigation into
samples [6,7]. The principle of SPD processes includes increasing the effect of SPD on electrical resistivity is very interesting and
the dislocation density by heavily uniform deformation, forming important.
of dense dislocation walls and acquiring ultrafined or nano-scaled Refining the grain size of useful metals such as low carbon steel
microstructure [8]. There are many researches on producing NS by SPD method is of great interest as the yield stress is significantly
materials using SPD and their mechanical properties. But, limited increased. This leads to an improvement in the strength to weight
works have been done on the variations of physical properties ratio, which is a desirable property for automobile industry. Also,
measuring the electrical resistivity changes of low carbon steel
sheets as a result of SPD process is very important. Among SPD
⇑ Corresponding author. Tel.: +98 21 66165227; fax: +98 21 66005717. methods that are now available [7,12–19], two major processes
E-mail address: mkazemi@sharif.edu (M. Kazeminezhad). that applicable for sheets are accumulative roll bonding (ARB)

0261-3069/$ - see front matter Ó 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.matdes.2011.02.032
F. Khodabakhshi, M. Kazeminezhad / Materials and Design 32 (2011) 3280–3286 3281

and constrained groove pressing. The process of ARB was invented 2. Material and methods
by Saito et al. [20,21], involves repetitive bonding between two
rolled plates and if perfect bonding is not accomplished, the In this research, as-received low carbon steel sheets with dimen-
bonding interface may reduce the mechanical properties of the sion of 84 mm  45 mm  3 mm were used to study the effects of
products. Thus, ARB is less considered feasible for severe plastic CGP process on grain refining and variation of electrical resistivity.
deformation of sheet metals. Constrained groove pressing for The chemical composition of this steel is shown in Table 1. Sche-
severe plastic deformation was initially proposed by Shin et al. matic of CGP dies are shown in Fig. 1. One pass of CGP that includes
[18]. The principle of groove pressing (GP) is that a material is four pressing stages is shown in Fig. 2 (stages 1–4). The pressings are
subjected to repetitive shear deformation under plastic strain performed such that the gap between the upper die and the lower
deformation condition by utilizing alternate pressings with asym- die is the same as the sample thickness, resulting in pure shear
metrically grooved dies and flat dies. As can be seen in Fig. 1, the deformation under plane strain condition at inclined regions of the
groove pressing is carried out such that the gap between the upper sample. Once the work piece is pressed between the grooved dies,
die and lower die is the same as the sample thickness and therefore under plane strain condition, an effective strain of 0.58 is imposed
the inclined region of the sample is subjected to pure shear defor- to the inclined regions while the flat areas undergo no deformation
mation under plane strain deformation condition [8]. Since this (Fig. 1(stage 1)). Then the work piece is removed from the dies and is
method has been recently invented, there are not many works on flattened by a set of flat dies, resulting in another 0.58 effective strain
it and more works should be carried out to examine the evolution in reverse direction which ends up in 1.16 strain for the deformed re-
of microstructure and mechanical properties of metals during this gions (Fig. 1(stage 2)). After the straightening, the specimen is ro-
process. Also, since the SPD of low carbon steel sheet is important tated 180° around the axis perpendicular to the plane of the sheet
and ARB has some disadvantages, in this study CGP method is used which ensures that the subsequent groove pressing (Fig. 1(stage
for imposing the severe plastic deformation on the low carbon 3)) and straightening (Fig. 1(stage 4)) impose an overall strain of
steel sheets. 1.16 to the undeformed regions. Then, a uniform strain of 1.16 has
In the previous work [22], mechanical properties improvement been imposed on the specimen. In this study, Teflon layers that
of low carbon steel sheets subjected to CGP have been investigated introduced in previous works [22,23] were used as lubricant be-
and it has been shown that this method can effectively increase the tween low carbon steel sheet and dies. Using the Teflon layers leads
strength and hardness of sheets. But, microstructure and some to impose the strain magnitude of 4.64 on the low carbon steel
physical properties such as electrical resistivity of low carbon steel sheets through four passes.
sheets during CGP process require more investigations. The microstructures of deformed sheets after CGP were investi-
In the present study, strains from 0 to 4.64 (each CGP pass im- gated using optical microscopy, X-ray diffraction and transmission
poses strain magnitude of 1.16) are imposed to the low carbon electron microscopy. In order to examine the microstructure with
sheets in order to produce a high strength nano-structured sheet. optical microscopy, the as-received sample was selected from the
Then, the microstructural characteristics of produced sheets are surface plane of specimen. For optical microscopy, samples were
investigated using XRD, TEM, and optical observations. XRD is em- ground on papers, polished and then etched in a solution of CH3OH
ployed to determine the grain size and to monitor the microstruc- containing 3% HNO3.
tural changes during SPD processes and TEM is used for verifying
the XRD results. The dislocation density of as-pressed sheets after Table 1
Chemical composition of low carbon steel sheet (wt.%).
each CGP pass is calculated from mechanical behavior of sheets.
Also, the effect of imposing strain on the electrical resistivity is Fe C Si Mn P S Cr Ni Mo
investigated using standard 4-point probe technique at room Base 0.0527 0.0229 0.203 0.006 0.0031 0.0088 0.0281 0.0024
temperature.

Fig. 1. Schematic of dies used through CGP process, left: grooving die, right: flattening die.
3282 F. Khodabakhshi, M. Kazeminezhad / Materials and Design 32 (2011) 3280–3286

Fig. 2. Four stages of one CGP pass.

To investigate the microstructure evolution of sheets during


CGP process, X-ray diffraction patterns and transmission electron
microscopy observations were used. XRD measurements were car-
ried out on a Philips X-ray diffractometer equipped with a graphite
monochromator using Cu Ka radiation and the results were ana-
lyzed using modified Williamson–Hall approach. Full-width at
half-maximum (FWHM) for all peaks was measured using the soft-
ware configured with the XRD system. The X-ray patterns of sam-
ples were achieved at a step width of 0.02°. For calibration of the
instrumental line broadening, a fully mixture of coarse TiC and
B4C powders was tested in the same condition.
For verifying of XRD results, the microstructural examination of
samples was performed using a transmission electron microscopy
operated at 100 kV. For TEM, discs having diameter of 3 mm and
thickness of 3 mm were cut from the three passes CGPed sheet.
Then, they were ground to a thickness of 0.2 mm and electro pol-
ished using a twin-jet polishing facility and a solution of 10% HClO4
and 90% CH3COOH. All of these discs were examined using a micro-
scope operating at 100 kV.
To measure the yield strength variations of low carbon steel
sheets after CGP process, tensile test was carried out. Tensile sam-
ples were prepared along longitudinal direction of the as-pressed
sheets with gage length of 32 mm according to the ASTM E8M
standard [24]. Tensile tests were conducted at room temperature
using an Instron tensile testing machine operating at a constant
Fig. 3. Schematic of 4-point probe configuration.
speed of cross-head and with an initial strain rate of 5  103 s1.
Electrical resistivity values of low carbon steel sheets for
as-received condition, one, two, three and four passes of CGP were ening have the advantage of averaging over a much larger area of
measured by standard 4-point probe technique at room tempera- the sample and ease of sample preparation [25]. X-ray line profile
ture. Schematic of 4-point probe configuration on the specimen analysis has been well used in studying the grain size, density and
is shown in Fig. 3. The four metal tips were part of an auto- arrangement of dislocations in deformed metals [27].
mechanical stage that travel up and down during measurements. Imperfections in nano-crystalline materials cause peak broad-
A high impedance current source was used to supply current ening compared with the Bragg peak that results from perfect
through the outer two probes; a voltmeter measured the voltage crystal diffraction. Grain size and lattice micro strain can be
across the inner two probes (see Fig. 3) to determine the sample accordingly determined by measuring the deviation of line profile
resistivity. Probe spacing in these experiments was s4 mm. Sam- from perfect crystal diffraction. In addition, the environment in a
ples for resistivity measurements were selected from the center of commercial diffractometer is not ideal and instrumental broaden-
sheets and the surface finishing treatment was carried out before ing arising from other effects, such as slit width, wavelength width
test. of the Ka1 and Ka2 lines, must be extracted in advance [25]. In prin-
ciple, the experimental profile is the convolution of the instrumen-
tal profile and the intrinsic profile (pure diffraction profile). The
3. XRD profile analysis intrinsic profile can be obtained by unfolding the experimental
profile.
It is of interest to characterize the grain size of NC materials The reciprocal-space variable, shown with S symbol, can be
processed via SPD approach both from the fundamental and per- identified as S ¼ 1=dhkl ¼ 2 sin h=kx , where dhkl is the distance be-
formance standpoints because their behaviors are intrinsically size tween hkl planes, h is the Bragg angle and kx is the wavelength of
dependent [25]. Transmission electron microscopy and X-ray dif- X-ray.
fraction are two basic methods for the grain size evaluation. Trans- When the size and strain broadening are simultaneously pre-
mission electron microscopy can provide a direct image from the sented, the separation of size and strain broadenings by the meth-
grain size distribution. However, grain overlapping leads to uncer- od of integral breadths can be performed based on explicit
tainty and the reliability also depends on whether the thin area is a assumptions as the shape of the broadening profile due to each
representative of the original microstructure of the entire sample effect. The profiles should be bell-shaped functions in mathematics
[25,26]. In contrast, the indirect methods based on XRD line broad- and hence it is often approximated as Cauchy or Gaussian
F. Khodabakhshi, M. Kazeminezhad / Materials and Design 32 (2011) 3280–3286 3283

functions. Like the extraction of instrumental broadening, assump-


tions are taken to relate the two components as the following
relationships [25,28]:

ðdSÞ2phy þ ðdSÞ2ins ffi ðdSÞ2exp ð1Þ

where (dS)phy, (dS)exp, and (dS)ins are the integral breadth of intrinsic
profile, experimental profile, and instrumental profile, respectively.
Typical XRD pattern of low carbon steel after two CGP passes is
shown in Fig. 4. As can be seen, the diffractions from three crystal-
line planes are more intense than those of others; (1 1 0), (2 0 0)
and (2 1 1). Therefore, in this study the diffractions of these three
peaks on all samples are considered to find the evolution of
microstructure.
All XRD measurements are based on Full-width at half-maxi-
mum for all peaks in S scale. Considering S – Intensity curves Fig. 6. The variation of ðdSÞ2phy versus S2 for steel sheet after fourth pass of CGP.
(Fig. 5) for severely deformed specimens and standard specimen,
(dS)phy for each specimen can be calculated.
Strain anisotropy is well known in literature as a non-mono- profiles, taking into account the shape of their decay, it is more
tonic increase of X-ray line broadening with diffraction order appropriate to introduce the notation [27]:
[27]. Several models have been suggested to account this effect;  2
however, these models lack a sound physical basis. A dislocation 0:9 c
ðdSÞ2phy ffi 
þ A 0 q S2 C ð3Þ
model has been recently suggested based on the anisotropic con- D
trast of dislocations in diffraction. It has been suggested that the 0
classical Williamson–Hall plot [27,29]: where A is one constant in the calculations. From this equation, it
 2 ! can be seen that using plot ðdSÞ2phy versus S2, the grain size of spec-
0:9 p M2d b2 c imens can be calculated (Fig. 6).
ðdSÞ2phy ffi þ q S2 C ð2Þ
D 2
c
where D, q and b are the average particle size, the average disloca- 4. Results and discussion
tion density and the modulus of the Burgers vector of dislocations.
Md is a constant depending on the effective outer cut-off radius of 4.1. Microstructural evaluation
dislocations. Since, Md can be only obtained from the tails of the
The microstructure of the as-received low carbon steel sheet
observed on the surface plane of sheet is shown in Fig. 7. The
as-received steel consists of approximately 6 vol.% pearlite (dark
contrast) and the remainder is ferrite (bright contrast). It is clearly
shown in Fig. 7 that the initial microstructure contains equiaxed
grains in size of 30 lm.
By analyzing the XRD patterns, evolution of low carbon steel
cell size during CGP process is calculated and shown in Table. 2.
As can be seen during first pass of CGP, the coarse grained low
carbon steel (with average grain size of 30 lm) is refined to a struc-
ture with cell size of 346 nm. However, after this rapid refinement,
the rate of refining is decreased and after fourth pass of CGP, the
cell size is about 230 nm.

Fig. 4. X-ray diffractogram of low carbon steel after fourth pass of CGP.

Fig. 7. Optical microstructure of as-received low carbon steel from specimen


Fig. 5. S – Intensity curve for low carbon steel after fourth CGP pass. surface.
3284 F. Khodabakhshi, M. Kazeminezhad / Materials and Design 32 (2011) 3280–3286

Table 2 4.2. Strength and dislocation density


The grain size value versus CGP pass number achieved by XRD approach.

CGP pass number Accumulative strain Cell/grain size (nm) The yield stress variations of the deformed sheets versus mag-
1 1.16 346 nitude of effective strain are shown in Fig. 9. The general trend that
2 2.32 265 can be found in Fig. 9 is that the yield strength of sample is in-
3 3.48 242 creased during deformation until first pass of CGP, however for
4 4.64 231 the other passes, strength drop is observed. The as-received sheet
has yield strength of 204 MPa. After one pass of CGP, yield strength
is increased from 204 MPa to 412 MPa. Increasing the strength of
material during SPD is common and arises from the work harden-
Dislocation theories can interpret this trend considering the
ing and grain refining mechanisms. Previous papers on CGP of cop-
relationship between imposed strain rate and rate of dislocation
per and aluminum explained the dropping phenomenon using two
generation obtained from the Orowan equation [30]. From this
theories; flow softening and micro cracking [23,32]. The achieved
relation, it can be concluded that the rate of dislocation density
strength values show a similar trend reported for aluminum and
generation is increased with increasing the resolved shear strain.
copper by researchers in previous works [8,16,18,23,33,34].
Since the cell size is proportional to inverse squared root of dislo-
As similar to other UFG materials, the tensile deformation
cation density [8,31], it seems that deformation can refine the
behavior of the present UFG low carbon steel are characterized
structure in a uniform manner. However, the second type of dislo-
by high strength and the absence of strain hardening [35]. Since
cation reactions during deformation that is called dynamic recov-
the UFG materials exhibit no strain hardening, its high strength
ery prohibits the steady rate of grain refinement. The main role
can not be explained by the dislocation pile-up mechanism
of dynamic recovery is dislocation annihilation and since the rate
[35,36]. However, as noted by Valiev et al. [35], the dislocation
of dynamic recovery is proportional to the material dislocation
bow-out model, which was often quoted for explaining the
density, the rate of dynamic recovery is increased through strain-
mechanical behavior of nano-crystalline materials, would be appli-
ing and causes to decrease the rate of grain refinement at large
cable to the present experimental results. In the dislocation bow-
strains. Therefore, it is acceptable to observe intensive grain refine-
out model [37], yielding occurs when the dislocation configuration
ment at the initial passes of CGP and a low rate of refinement at the
reaches semicircle and the critical stress for such condition is
following passes.
approximated by an expression of:
Fig. 8 shows the TEM microstructure of the groove pressed low
    
carbon steel after three CGP passes. As can be seen in this figure, Gb 3m L m
cellular structure is formed in third pass. Comparing the TEM
scritical ¼ 1 ln 1þ ð4Þ
2pLð1  mÞ 2 b 2
observation with the results of XRD analysis (that presented in
Table 2) shows that both approaches determine the same range where G is the shear modulus, b is the burgers vector, m is the Pois-
of cell size for CGPed low carbon steel. Also, comparing the TEM son’s ratio and L is the average dislocation length. For the grain size
1
observations, reported by Langdon et al. [12], for the equal channel larger than 100 nm, L is equivalent to q2 where q is the dislocation
angular extrusion (ECAE) of the same composition steel with the density [38]. With the aid of Eq. (4), the yield stress of UFG materi-
achieved results of XRD analysis shows that both ECAE and CGP als can be expressed as:
processes have similar effect on grain size evolution of low carbon
rYS ¼ r0 þ Mscritical ð5Þ
steel.
where r0 is the friction stress and M is the Taylor factor. By using
Eqs. (4) and (5), and yield strength curve (Fig. 9), dislocation density
of the CGPed steel is estimated as presented in Fig. 10 using the fol-
lowing values; G = 78 GPa, b = 2.48  1010 m, m = 0.33, M = 2.78 for
BCC structure and r0 = 76 MPa [39].
As can be seen in Fig. 10, the dislocation density value of low
carbon steel sheets is rapidly increased through first pass of CGP
from 1.37  1013 m2 to 1.6  1014 m2. However in the following
passes, the rate of dislocation density increscent is reduced and for
the three last passes, a drop is observed. Increasing the dislocation

Fig. 8. TEM micrograph of the low carbon steel after third pass of CGP. Fig. 9. Yield strength variation of low carbon steel sheets during CGP process.
F. Khodabakhshi, M. Kazeminezhad / Materials and Design 32 (2011) 3280–3286 3285

electrical resistivity increscent is reduced and also it can be ob-


served that the resistivity of four passes deformed sample is higher
than that of three passes deformed sample and is about
106.06 lX cm. This trend can be interpreted by considering the ef-
fects of grain boundaries and dislocations on electron scattering.
The contribution of different types of defects into the electrical
resistivity of metals such as low carbon steel (qFe) can be estimated
by data of some references [40,41]. Impurities, dislocations and
grain boundaries are the main defects determining the value of
electrical resistivity, and resistivity of materials can be partitioned
into the contributions of three main scattering mechanisms [11] as
follows:

q ¼ qimpurities þ qdislocations þ qgrainboundaries þ ::::: ð6Þ

Fig. 10. The dislocation density of severely deformed sheets versus strain.
where q is the total electrical resistivity, qimpurities is resistivity of
impurities, qdislocations is due to dislocations resistivity and
qgrain-boundaries is the grain boundaries effect.
density during SPD is common and its reason can be explained by The change in electrical resistivity caused by scattering on the
considering the relation between imposed strain rate and rate of grain boundaries is expressed by:
dislocation generation when the Orowan equation is considered
X
on a large time scale [30]. But, decreasing the dislocation density dq ¼ qb S ð7Þ
in last passes is due to the role of dynamic recovery on dislocations
annihilation. These phenomena can influence on the dislocation
density variation through CGP with similar trend that those affect where qb is the specific electrical resistivity of grain boundaries;
the grain refinement mechanism in previous section. Rate of dy- S ¼ 2m is the total specific surface of all grains in the unit of volume,
namic recovery is increased with increasing the CGP pass number m is the average number of intersections of linear intercept with
and causes to decrease the dislocation density with straining grain boundaries per 1 cm. Also, the changes in electrical resistivity
through last passes. The trend of dislocation density variation that due to scattering from dislocations can be expressed as:
measured by this approach is reliable. Dislocation density calcu-
lated by this method is lower than real dislocation density of mate- dq ¼ qD  ND ð8Þ
rial, because all kinds of dislocations are not considered in the
model. Also, some of mechanical phenomena such as micro crack- where qD is the value of resistivity change per unit length of dislo-
ing can reduce the strength of metals and therefore this model can cation and ND is the concentration of dislocations (dislocation den-
decrease the magnitude of dislocation density, but in fact this phe- sity). In one research on copper, it has been shown that the
nomena can not decrease the total dislocation density of materials. influence of grain boundaries resistivity on electrical resistivity is
significant and it is more than 50% [11]. Also, the influence of solid
4.3. Electrical resistivity variation solution elements on electrical resistivity is negligible, if a large part
of impurities is in form of fine precipitation (which influences the
The aim of this study is to show the effects of ultrafine structure specific resistivity of grain boundaries and stabilization of the dislo-
and dislocation density of low carbon steel sheets on electrical cation structure). The change in resistivity due to the dislocations is
resistivity of them. The value of electrical resistivity as a function defined by the uniformity of their distribution. The presence of fully
of CGP pass number and effective strain is shown in Fig. 11. As recrystallized grains with low local value of resistivity in strain
can be seen, imposing one pass of CGP can rapidly increase the hardened materials can lead to the decrease of the effective resistiv-
resistivity of low carbon steel sheets from 57.44 lX cm to ity [11,42–44].
97.22 lX cm. However in the following passes, the rate of As shown in two previous sections, due to imposing of the SPD
to low carbon steel sheets, the dislocation density is increased by
heavily uniform deformation and coarse-grained ferritic micro-
structure is refined to nano-structure. Refining the microstructure
causes to increase the total surface of all grains. Since grain sur-
faces and dislocation density are increased with increasing the
CGP pass number, by considering Eqs. (7) and (8) increasing the
electrical resistivity with increasing the pass number up to
100% is reasonable as shown in Fig. 11. However, after rapid
increasing in electrical resistivity one pass CGPed specimen, the
rate of resistivity variation is decreased. This can be attributed to
the effect of dynamic recovery on dislocation annihilation and
decreasing the rate of grain refinement at large strains. It should
be noted that in Fig. 11, the electrical resistivity of four passes de-
formed sample is increased compared with that of previous pass.
Since deformation through fourth pass can generate some micro
cracks on the sheet surface (due to friction effect in interface of
sheet and dies), the air gaps can be as obstacles for electrons trans-
Fig. 11. The variation of electrical resistivity with CGP pass number and effective port or scattering source of electrons which lead to increase of the
strain. electrical resistivity.
3286 F. Khodabakhshi, M. Kazeminezhad / Materials and Design 32 (2011) 3280–3286

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